Born Victoria L‹pez Cima in Barcelona in 1923, De los Angeles studied at the Barcelona Conservatory and made her operatic debut at the city's Gran Teatre del Liceu in 1945, singing the Countess in Le nozze di Figaro. She won the Geneva International Vocal Competition in 1947, and debuted with the BBC in 1948, with the Paris Op_ra in 1949, at the Salzburg Festival, Covent Garden, La Scala, and Carnegie Hall in 1950, and at the Metropolitan Opera in 1951.

De los Angeles's signature role was Carmen, a part she sang many times; her 1959 recording of the opera, conducted by Thomas Beecham, is considered one of the best ever made.

In the 1960s, she shifted her focus to concert appearances, specializing in French, German, and Spanish art songs. She was an active performer into the 1990s, singing at the closing ceremonies of the Olympic Games in Barcelona in 1992.