Her duet with Freddie Mercury became the signature song of the Barcelona Olympics in 1992.
According to news agency Efe, Montserrat Caballé had been suffering from health complaints for some time and was admitted to hospital in Barcelona last month.
With a 50-year career, Montserrat Caballé had stints with the Basel Opera and Bremen Opera before her international breakthrough in 1965 in Lucrezia Borgia at Carnegie Hall in New York.
Montserrat Caballé went on to perform with the Metropolitan Opera, San Francisco Opera and Vienna State Opera, appearing opposite the likes of Luciano Pavarotti and Placido Domingo.
The song Barcelona was first released in 1987 and later became an anthem for the city’s 1992 Olympics, the year after Freddie Mercury died. She sang at the opening ceremony with Placido Domingo and José Carreras.
Montserrat Caballé was born in Barcelona, and at the age of nine was accepted for training at the city’s Conservatori Liceu.
She graduated in 1953, and went to Italy, where she sang some minor roles.
Montserrat Caballé’s career advanced rapidly after a successful appearance as Mimi in La Bohème at the Basel Opera. In 1965 she made a triumphant debut in the US, taking over the title role – at short notice – of Donizetti’s Lucrezia Borgia at Carnegie Hall.
The singer’s performance brought widespread praise for the beauty of her voice and her dramatic interpretation, and established her as an international star.
Montserrat Caballé’s career was dogged by ill health. In 1985, she spent three months in hospital with a brain tumor, and had treatment for heart trouble in 1993.
In 2015, Montserrat Caballé was given a six-month suspended prison sentence for tax fraud.
According to Spanish media, plans are being made for a funeral in Barcelona on October 8.
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