She starred opposite Pedro Armendáriz, her favorite actor, in Dos hijos desobedientes (1960). Greatly admired by audiences for her beauty and talent, she became one of the most popular Mexican performers of the 1960s. Her last appearances were in the telenovelas El dolor de amar (1966), in which she played a villain for the first time, and Felipa Sánchez, la soldadera (1967), in which the press declared she created “an unforgettable character” as the title role.
Elvira Quintana, who never married, suffered from pancreatic problems and renal failure during her last months. She died of a stroke on 8 August 1968, in Mexico City; she was survived by her mother, Alejandra Molina, and her two siblings, Juana Quintana Molina and José Díaz Molina. She was interred at the Panteón Jardín on 9 August.
A street in Montijo, her hometown, is named after her.