With the arrival of talkies, Vélez appeared in a series of Pre-Code films like Hell Harbor (directed by Henry King), The Storm (1930, directed by William Wyler), and the crime drama East Is West opposite Edward G. Robinson (1930). In 1931, she appeared in her second film for Cecil B. DeMille, Squaw Man, opposite Warner Baxter, and in Resurrection, directed by Edwin Carewe. In 1932, Vélez filmed The Cuban Love Song (1931), with the popular singer Lawrence Tibbett. That same year, she had a supporting role in Kongo (a sound remake of West of Zanzibar), with Walter Huston. She also starred in Spanish-language versions of some of her movies produced by the Universal Studios like Resurrección (1931, the Spanish version of Resurrection), and Hombres en mi vida (1932, the Spanish version of Men in Her Life). Vélez soon found her niche in comedy, playing beautiful, but volatile, characters.
After her breakup with Cooper, Vélez began a short-lived relationship with actor John Gilbert. They began dating in late 1931, while Gilbert was separated from his third wife Ina Claire. Rumors of an engagement were fueled by the couple, but Gilbert ended the relationship in early 1932, and attempted to reconcile with Claire.