Ashford and Simpson met in a church choir and penned a string of hits including You're All I Need To Get By and Chaka Khan hit, I'm Every Woman.
They also had a hit themselves in the 1980s with Solid (As A Rock).
Ashford moved from his native South Carolina to New York to pursue a music career in the early 1960s.
Simpson later inscribed "Nick Ashford slept here" on the park bench he slept on in the city's Bryant Park, when he first came to New York and was homeless.
The couple's breakthrough hit was Ray Charles's Let's Get Stoned in 1966.
Their other hits include Ain't Nothing Like The Real Thing, one of several tracks written for duo Marvin Gaye and Tammi Terrell, and Diana Ross's first solo single, Reach Out and Touch (Somebody's Hand).
The pair were inducted into the Songwriters Rock and Roll Hall of Fame in 2002.
"I'm so sad that he's gone," Alicia Keys said in a tribute posted on Twitter: "What a legacy of infectious music."
"His music is unmatched in terms of great songwriting," said Verdine White of Earth, Wind and Fire.
"They had magic and that's what creates those wonderful hits, that magic. Without those songs, those artists wouldn't have been able to go to the next level."
Ashford and Simpson are also credited as co-writers on Amy Winehouse's track, Tears Dry On Their Own, which contains a sample from Ain't No Mountain High Enough.
Ashford is survived by his wife and their daughters Nicole and Asia. Funeral arrangements have yet to be announced.
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