After a hiatus of several years, Moore returned to Hollywood under contract to Columbia Pictures, for whom she made six films. In the 1934 film One Night of Love, her first film for Columbia, she portrayed a small-town girl who aspires to sing opera. For that role she was nominated for the Academy Award for Best Actress in 1935. She starred in 1936 as Empress Elisabeth of Austria in Josef von Sternberg's production The King Steps Out.
By this time, she was so popular that MGM was able to insist on equal billing for Moore in a projected film with Maurice Chevalier, who had always enjoyed solo star billing up until then. Chevalier felt so deeply about this blow to his status that he quit Hollywood and the film was never made.
A memorable highlight of When You're in Love (1937) was a comic scene in which Moore donned flannel shirt and trousers and joined a 5-man band for a flamboyant rendition of Cab Calloway's "Minnie the Moocher", complete with gestures and "hi-de-ho's", but with the lyrics slightly altered to conform with Hollywood sensibilities. Also, she performed the popular Madama Butterfly duet "Vogliatemi bene" with American tenor Frank Forest in the 1937 film I'll Take Romance.
The last film that Moore made was Louise (1939), an abridged version of Gustave Charpentier's opera of the same name, with spoken dialog in place of some of the original opera's music. The composer participated in the production, authorizing the cuts and changes to the libretto, coaching Moore, and advising director Abel Gance. This production also featured two renowned French singers: dramatic tenor Georges Thill and basse cantante André Pernet.