The influential R&B figure passed away following a concert he performed in Spain, said The Hollywood Reporter.
Rescue workers were called to Toussaint's hotel early Tuesday morning and managed to revive him after he suffered a heart attack, Madrid emergency services spokesman Javier Ayuso said.
But Toussaint stopped breathing during the ambulance ride to a hospital, and efforts to revive him again were unsuccessful, Ayuso said. Toussaint performed Monday night at Madrid's Lara Theater.
"He was a legend in the music world. You always saw Allen with a coat and tie and wearing sandals," said Quint Davis, who produces the New Orleans Jazz and Heritage Festival.
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The pianist-songwriter was born in New Orleans and went on to become one of the city's most celebrated performers.
He worked as a producer for the New Orleans-based Minit Records in 1960 before being drafted in the Army for two years.
He later created his own recording studio in 1973 with fellow songwriter Marshall Sehorn, called Sea-Saint Studio. There he worked with musicians including Paul Simon, Paul McCartney, Patti LaBelle, the late Joe Cocker and Elvis Costello.
Toussaint has hundreds of hits to his name and received the Recording Academy Trustees Award at the 2009 Grammy Awards. He penned the 1966 Lee Dorsey classic "Working in a Coal Mine" and produced Dr John's 1973 hit "Right Place, Wrong Time" and 1975's "Lady Marmalade" by the vocal trio Labelle.