SS career
After the war, Waldeck-Pyrmont studied agriculture. On 1 November 1929, he joined Adolf Hitler's Nazi Party, becoming a member of the Schutzstaffel (SS) on 2 March 1930. He was immediately appointed adjutant to Sepp Dietrich, before becoming Reichsführer-SS Heinrich Himmler's adjutant and staff chief in September 1930.
Waldeck-Pyrmont was elected to the Reichstag in March 1933 on the electoral list of the Nazi Party. At the November 1933 election, he was returned as a deputy for electoral constituency 23, (Düsseldorf West) and retained this seat until the final days of the Nazi regime. Also in 1933, he was promoted to the rank of SS lieutenant general. He was appointed in 1938 to the post of Higher SS and Police Leader for Weimar. In this position he had supervisory authority over Buchenwald concentration camp.
Buchenwald had first caught the attention of Waldeck in 1941 when, glancing over the camp's death list, he came across the name of Walter Krämer, a head hospital orderly at Buchenwald. He recognized it because Krämer had successfully treated him in the past. Waldeck investigated the case and discovered Karl-Otto Koch, the camp's commandant, had ordered both Krämer and Karl Peix (a hospital attendant) killed as "political prisoners" because they had treated him for syphilis, a fact Koch wished to keep secret. Waldeck also received reports that a certain prisoner had been shot while attempting to escape. By that time, Koch had been transferred to the Majdanek concentration camp in Poland, but his wife, Ilse, was still living at the Commandant's house in Buchenwald. Waldeck ordered a full-scale investigation of the camp by Georg Konrad Morgen, an SS major who was a judge in a German court. Throughout the investigation, more of Koch's orders to kill prisoners at the camp were revealed, as well as evidence of embezzlement of property stolen from prisoners. It was also discovered that the prisoner who was "shot while trying to escape" had been told to get water from a well some distance from the camp, then was shot from behind; he had also helped treat Koch for syphilis. A charge of incitement to murder was lodged against Koch by Waldeck-Pyrmont and Morgen, to which later was added a charge of embezzlement. Other camp officials were also charged, including Ilse Koch. The trial resulted in a death sentence for the Commandant, who was executed by firing squad on 5 April 1945. Morgen was convinced that Ilse Koch was guilty of sadistic crimes, but could not prove the charges against her; she was detained by German authorities until early 1945.
Adolf Hitler appointed Waldeck-Pyrmont a member of the Ordnungspolizei (uniformed police) in April 1941 and, a year later, he was appointed High Commissioner of Police in German-occupied France. One of his first acts in his new role was ordering French hostages to be placed on German troop trains, to discourage sabotage attempts on them. He was made a general in the Waffen-SS in July 1944.