Alou, who played on four teams in his 15-year career, won both of his World Series titles as a member of the Oakland Athletics in 1973 and 1974.
"We are heartbroken by the passing of Jesús Alou," the A’s said in a statement.
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"He was a key member of our World Series-winning teams in 1973 & 74 and will forever be a member of the A’s family."
Alou spent the first six years of his career with the San Francisco Giants, hitting .279 with 18 home runs in 633 games.
On September 15, 1963, Alou made history when he and his two brothers, Felipe and Matty Alou, appeared in the same outfield together, according to MLB Network.
"The San Francisco Giants are saddened to learn of the passing of former outfielder Jesús Alou," the Giants posted to Twitter.
"Our thoughts, prayers and deepest condolences go to the Alou family, his friends and all those whose lives he touched."
Alou went on to play with the Houston Astros and the New York Mets, retiring in 1979 with a career batting average of .280.
Alou began working for the Boston Red Sox in 2002 as a scout and directed the team’s academy in the Dominican Republic.
"We are deeply saddened by the passing of Jesús Alou," the Red Sox said.
"A 2x World Series champion, with over 60 years in baseball as a player, coach, scout, & ambassador, Jay was the patriarch of the Red Sox Dominican Academy & Lindos Sueños, bringing together communities within Red Sox Nation."