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Téa Leoni as Elizabeth McCord, the U.S. secretary of state and later the president of the United States. Elizabeth spent twenty years as a CIA analyst before retiring to become a professor of political science at the University of Virginia. She is appointed secretary of state by her former CIA boss, President Conrad Dalton, to replace Secretary of State Vincent Marsh, who died in a plane crash. She later succeeds Dalton as president.

Tim Daly as Henry McCord, Elizabeth's husband of 25 years and later the first gentleman of the United States. A theology professor and former Marine Corps aviator during Operation Desert Storm, he is hired by the National Security Agency, which employs him as an operative in combating religious extremism. At the end of the third season, Henry is appointed as the head of the CIA's Special Activities Division.

Bebe Neuwirth as Nadine Tolliver (seasons 1–4), Elizabeth's chief of staff. Nadine had a six-year affair with the late secretary of state Vincent Marsh, beginning when he was a senator from Illinois. Originally suspicious and resentful of the new secretary of state, Tolliver soon learns to trust McCord, and the two cultivate a strong working relationship. In the first season, Nadine romances NASA Administrator Glenn and later falls into a relationship with political consultant Mike Barnow. In the fourth season, Nadine retires from the State Department to spend more time with her family in San Francisco when her son Roman tells her that he is going to have a child.

Željko Ivanek as Russell Jackson, the White House chief of staff for President Dalton. McCord appoints him as her chief of staff as well, 98 days into her presidency. His objective of keeping the president politically secure often results in confrontation with McCord due to her unorthodox diplomatic techniques.

Erich Bergen as Blake Moran, Elizabeth's personal assistant and the only member of her staff as secretary of state that she hired rather than inherited. In the fifth season, McCord fires him, only to rehire him as her new assistant policy advisor.

Patina Miller as Daisy Grant, Elizabeth's press coordinator. Daisy briefly dates speechwriter Matt Mahoney in the first season. In the third season, she dates "Kevin" from the Bureau of Budget and Planning, who turns out to be an undercover CIA operative investigating the State Department. After he is killed in a weapons-trafficking conspiracy, Daisy learns she is pregnant with his child. In the fourth season, Daisy gives birth to their daughter, Joanna Grant.

Geoffrey Arend as Matt Mahoney, Elizabeth's speechwriter. Matt briefly dates Daisy in the first season; the two are implied to have rekindled their relationship by the end of the series.

Wallis Currie-Wood as Stephanie "Stevie" McCord, Elizabeth and Henry's daughter and oldest child. Stevie attended Lovell University and Georgetown University, and later applied to Harvard Law School. She serves as an intern to Russell Jackson and was previously engaged to Jareth Glover. In the fourth season, Stevie begins a secret relationship with Dmitri Petrov while he is undercover, placing them both in peril. In the series finale, Stevie and Dmitri marry in a ceremony officiated by former President Dalton.

Kathrine Herzer as Alison McCord, Elizabeth and Henry's younger daughter.

Evan Roe as Jason McCord, Elizabeth and Henry's only son and youngest child. Jason is a leftist and self-proclaimed anarchist who is generally critical of his mother's political views but protective of her personal reputation.

Keith Carradine as Conrad Dalton (seasons 2–6; recurring season 1), the President of the United States. Conrad served in the United States Marine Corps as a second lieutenant during the Vietnam War and was the Director of the Central Intelligence Agency during Elizabeth's career at the CIA. In the third season, Dalton is re-elected as an independent candidate after failing to secure his party's nomination, in part due to a controversial change in policy championed by Elizabeth. He offers Elizabeth the role of vice president during his campaign, but eventually taps Teresa Hurst for the position instead.

Sebastian Arcelus as Jay Whitman (seasons 3–6; recurring seasons 1–2), Elizabeth's chief of staff and (formerly) senior policy advisor. In the third season, Jay and his wife Abby (Stephanie J. Block) separate because of his punishing work schedule; she retains custody of their daughter, Chloe. Jay is promoted to chief of staff in the fourth season. In the fifth season, while stuck at Shannon Airport in Ireland due to a volcanic eruption in Iceland, Jay meets noted Dutch chess player Annelies De Runnow (Marissa Neitling). They develop a mutual attraction after many hours at the airport, and agree to start a long-distance relationship. When Elizabeth decides to run for president, Jay initially passes on the chance to serve as her chief of staff in order to start a life with Annelies. Elizabeth later rehires Jay as her chief of staff.

Sara Ramirez as Kat Sandoval (seasons 4–5), Elizabeth's policy advisor and former chief of staff to the U.S. ambassador to the United Nations.

Kevin Rahm as Michael "Mike B." Barnow (season 6; recurring seasons 1–5), a sarcastic political consultant and operative who occupies several positions among the departments of the U.S. cabinet. Barnow is a Rhodes scholar who is said to have left a brilliant legal career for a political career that was cut short by a scandalous divorce. His unofficial role as an advisor to Elizabeth earns him a reputation as her 'hatchet man'. Elizabeth later appoints him as her campaign manager during her presidential run. Following her victory, she appoints him as her White House chief of staff. After her first 100 days in office, Elizabeth asks him to remain as chief of staff, but he refuses and instead chooses to serve as counselor to the president. Mike is rarely seen without his beloved Australian cattle dog Gordon.

Recurring

Johanna Day as Ellen Hill, a retired admiral serving as national security advisor. She was the first female chair of the joint chiefs of staff prior to her appointment as national security advisor.

Tony Plana as Ed Parker, an admiral and member of the joint chiefs of staff.

Francis Jue as Ming Chen, minister of foreign affairs of the People's Republic of China and Elizabeth's Chinese counterpart.

Mandy Gonzalez as Lucy Knox, President Dalton's aide.

Mike Pniewski as Gordon Becker, the U.S. secretary of defense.

Jason Ralph as Harrison Dalton (seasons 1–2), the son of President Dalton and a long-time friend of Stevie McCord. Harrison suffers from drug addiction; in the fourth season, it is revealed that he is back in rehab.

Matt Meinsen as Matt (seasons 1–5), Elizabeth's lead diplomatic security service agent.

Cotter Smith as Darren Hahn (seasons 1–2), President Dalton's first national security advisor.

Patrick Breen as Andrew Munsey (season 1), the director of the CIA and a protégé of President Dalton.

Marin Hinkle as Isabelle Barnes (season 1), a CIA analyst and Elizabeth's close friend, who assists the McCords with their investigation into the death of Secretary of State Vincent Marsh.

Nilaja Sun as Juliet Humphrey (season 1; guest season 3), a former CIA analyst and friend of Elizabeth and Isabelle.

Usman Ally as Zahed Javani (season 1), minister of foreign affairs of Iran and Elizabeth's Iranian counterpart.

Dion Graham as Fred Cole (season 1), head agent of the Bureau of Diplomatic Security and Elizabeth's principal bodyguard.

Josh Hamilton as Arthur Gilroy (season 1), Stevie's 39-year-old employer and boyfriend.

Anna Deavere Smith as Mary Campbell (season 1), the U.S. attorney general.

Yorgo Constantine as Anton Gorev (seasons 1–2), minister of foreign affairs of Russia and Elizabeth's Russian counterpart.

Clifton Davis as Ephraim Ware (seasons 2–6), the director of national intelligence.

Julian Acosta as Craig Sterling (season 2), a former department of defense official and rival of Elizabeth's who becomes national security advisor in the second season, much to Elizabeth and Russell's dismay.

Alex Fernandez as Mark Delgado (season 2), the vice president of the United States.

Angela Gots as Maria Ostrova (season 2), president of Russia and widow of late Russian president Pavel Ostrov.

Leslie Hendrix as Louise Cronenberg (season 2), the U.S. attorney general.

Jill Hennessy as Jane Fellows (season 2), Henry's Defense Intelligence Agency superior and a member of Murphy Station, the first Hizb-al Shahid task force.

Kobi Libii as Oliver Shaw (season 2; guest season 3), a cybersecurity coordinator. Shaw investigates the cyberattack against Air Force One and becomes romantically involved with Daisy Grant in the second season.

Chris Petrovski as Dmitri Petrov (seasons 2, 4; guest seasons 3, 5–6), a 24-year-old Russian Army captain who attends the National War College. Dmitri is recruited by Henry McCord on behalf of the Defense Intelligence Agency, and becomes an American spy in exchange for his sister Talia to receive cancer treatment in Stockholm. Dmitri is eventually discovered and captured by the Russians, and is later returned to the United States as part of a prisoner exchange. Dmitri feels abandoned by Henry following his capture, and begins to act bitter towards him. He is eventually placed into a witness protection program and is sent to Phoenix under the alias "Alexander Mehranov". In the fourth season, Dmitri is recruited by the CIA as an analyst; he eventually begins a romantic relationship with Stevie, and the two are married in the series finale.

Masha King as Talia Petrov, Dmitri's sister who is placed into witness protection alongside her brother.

Carlos Gómez as Jose Campos (seasons 2–3), a Murphy Station (Hizb-al Shahid task force) member. While he initially has a combative relationship with Henry, the two eventually become friends.

Tonya Pinkins as Susan Thompson (seasons 3–6), assistant secretary for the Bureau of African Affairs and, as of the end of the fifth season, secretary of state under the McCord administration. She serves as a key voice in bringing African issues to Elizabeth's attention, and encourages her to intervene in the Angolan election in the third season.

J. C. MacKenzie as Sam Evans (season 3), the governor of Pennsylvania and eventual presidential nominee for Dalton's party. Evans is particularly vindictive during the campaign and, following Dalton's victory, threatens to have the vote overturned due to a little-known law he claims Elizabeth broke. He is manipulated into accepting the terms of the vote, however, after Russell Jackson threatens to expose his possession of a gene that makes him likely to develop early-onset Alzheimer's disease.

René Auberjonois as Walter Novack (seasons 2–6), a state department analyst with the Bureau of International Security and Nonproliferation.

Christopher O'Shea as Jareth Glover, Stevie's upper-class English fiancé. Jareth gave up a fellowship at Oxford University to be with Stevie after she had trouble adjusting to life in England; the couple eventually breaks up in the fourth season.

Justine Lupe as Ronnie Baker (seasons 3–6), a United States Army Captain seconded from United States Cyber Command who assists Elizabeth on several occasions.

Eric Stoltz as Will Adams, Elizabeth's younger brother and a member of Doctors Without Borders.

Jordan Lage as Kohl, a United States Army general.

Sam Breslin Wright as Dylan Larson, an ex–Army Ranger and CIA operative.

Christine Garver as Molly Reid, a CIA operative who started her career as a field agent in Chechnya. She is pregnant from the beginning of the fourth season.

Tracee Chimo as Nina Cummings, Elizabeth's assistant who takes over from Blake after he vacates the position. In season six she begins working at the White House as Russell's assistant.

Wentworth Miller as Senator Hanson (season 6), a senator leading the congressional investigation into poll fraud accusations made against Elizabeth's presidential campaign.

Criticism

Three women have served as United States Secretary of State to date: Madeleine Albright from 1997 to 2001 under Bill Clinton, Condoleezza Rice from 2005 to 2009 under George W. Bush, and Hillary Clinton from 2009 to 2013 under Barack Obama. Shortly after the series' debut, Fox News asked if the show served as a campaign ad supporting Hillary Clinton, but quoted the Los Angeles Times saying the lead character was "no Hillary knock-off" and a New York publicist calling the casting of a woman "simple business and smart on CBS' behalf." Conservative activist organization Culture and Media Institute said "The connections in the show between Elizabeth and Hillary are clear, from the blond hair to the pantsuits."

When the trailer of the 15th episode of the third season titled "Break in Diplomacy" was released showing McCord responding to unwanted sexual advances by fictional Philippine president Datu Andrada by punching Andrada in the face, the series became controversial in the Philippines. Viewers noticed parallels between Andrada and real-life Philippine president Rodrigo Duterte, who was known for making inappropriate and sexist remarks. The Philippine Embassy in Washington published a statement protesting the negative depiction of the presidential character on its Facebook page.

The fourth-season premiere, "News Cycle", led to a protest from East Timor's Minister of State José Ramos-Horta, a Nobel Peace Prize laureate. He said, "It is a slander against a country that only shows ignorance and racism." The show used the border dispute between Australia and East Timor in the Timor Sea as background story. (The dispute is transferred in the TV show to the South China Sea, although neither Australia nor East Timor borders it). East Timor is shown as a country controlled by a Mexican drug cartel and used for the shipment of drugs. Secretary McCord asks China to take measures to prevent the leader of the drug cartel from making a narco-state out of East Timor.

In the fourth episode of the first season, "Just Another Normal Day", the series used stock footage shot in Hoi An, Vietnam, but noted the location as Fuling, China. This caused anger among the Vietnamese government, who said that the episode "offended Vietnam's sovereignty and territorial integrity". Soon after, the Department of Radio, Television and Electronic Information of the Ministry of Information and Communications of Vietnam ordered a ban on the series, and asked Netflix to remove the series from the Vietnamese version of Netflix.

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