Canadian Nestor and Frenchwoman Mladenovic, the eighth seeds who were runners-up at last month's French Open, dropped the first set to the Brazilian and American pairing and saved two match points in the third set before claiming their first grand slam title together.
Wimbledon singles champion Marion Bartoli, a close friend of Mladenovic's, watched the match from the stands before heading off for the champions ball.
It was the 40-year-old Nestor's third grand slam mixed doubles title and he has also won eight major men's doubles crowns, including two at the All England Club, and the 2000 Olympic gold medal.
The 39-year-old Raymond has won four grand slam titles in women's doubles and seven in mixed, including last year's crown at Wimbledon in partnership with compatriot Mike Bryan who won the men's doubles title with his brother Bob on Saturday.
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- Marion Bartoli