2018–present: Continued acting career and labels transition
In 2018, Jung was cast as the female lead in OCN's crime action drama Player, as Cha Ah-ryung, a highly skilled driver who ran away from orphanage. At the press conference for the drama, Jung stated that she learned how to ride a motorcycle in order to do her own stunts.
In 2019, Jung and her sister Jessica filmed their second reality show in the United States where they traveled across their homeland, exploring fashion, music, and culture while reminiscing about their childhood memories, titled Jessica & Krystal: US Road Trip which was released in 2021. The same year, she made her film debut in the independent romance More Than Family, playing To-il, a pregnant college student searching for her estranged father. She also starred in the Netflix-released romantic comedy Sweet & Sour, marking her commercial film debut.
In 2020, Jung was cast in OCN's military cinematic drama Search, where she played an elite army officer. The drama premiered on October 17, 2020. After reports began swirling of Jung departing SM Entertainment, SM responded that their contract with her would expire by the end of August 2020, and they were in discussions with her for a possible renewal. Krystal's departure from SM was officially announced in October 2020 and signed with H& Entertainment as her new agency.
In 2021, Jung starred in KBS2's drama Police University, playing Oh Kang-hee, a freshman at Korean National Police University, alongside Cha Tae-hyun and Jinyoung.
In 2022, Jung starred alongside Kim Jae-wook in the KBS2's romantic-comedy Crazy Love, playing Lee Shin-ah, a quiet but capable secretary whose life takes an unexpected turn. For her performance, she received the "Popularity Award", at the 2022 KBS Drama Awards.
In 2023, Jung starred in Cobweb, a period black comedy-drama film directed by Kim Jee-woon. It was premiered in the non-competitive section at the 2023 Cannes Film Festival. She received the "Best New Actress" award at the 33rd Buil Film Awards, and the "Best Supporting Actress" award at the Chunsa Film Art Awards 2023 for the role.
In February 2024, Jung released cover song of Leila Hathaway's "I'm Coming Back" through SoundCloud and also confirmed to join the label Beasts & Natives (BANA). Later in the same year, she made a special appearance in The Player 2: Master of Swindlers, the sequel to the 2018 drama Player. in which she starred as Cha Ah-ryung.
In January 2025, Jung was confirmed to star in the film Audition 109, co-directed by Jung Woo and Oh Seong Ho. In March 2025, Jung was selected as the ambassador for French Film Week, which was scheduled to take place from April 4 to 13. During a Q&A session following a general screening of the film Suspended Time, she revealed that she had been preparing for her solo album.
In April 2025, Jung starred as a special guest role in the fantasy romance drama Way Back Love as a senior grim reaper. The episode premiered on April 15.
In July 2025, it was confirmed that Jung would star in the tvN drama Mad Concrete Dreams alongside Ha Jung-woo, Im Soo-jung, Kim Jun-han, and Shim Eun-kyung. She is set to play Jeon Yi-kyung, a character who assists her mother's real estate business. The drama is scheduled to air in the first half of 2026.
On November 6, 2025, Jung announced through her agency BANA's official YouTube channel, released episode 1 of her solo album production series Charging Crystals and announced would release her solo album's first single "Solitary" on November 27.