He followed that with three consecutive seasons of batting better than .330, finishing third, second and fourth among NL leaders from 1967-69. He led the NL with 231 hits and 41 doubles in 1969.
"He'd hit balls in the gap and run for two days," said Joe Amalfitano, a teammate and opponent in the 1960s.
"One day at Candlestick he showed bunt early, then slapped at the ball. It took one, big high hop over the third baseman and went for a triple."
Alou played six seasons after being traded from Pittsburgh to St. Louis prior to the 1971 season, batting better than .300 in two more seasons.
He finished with the Padres in 1974 having played in 15 Major League seasons, having also played for the A's and Yankees. He had a career .307 batting average with 156 stolen bases and 1,777 hits, a total that included 50 triples.
In 1962, in the third game of a three-game playoff series to determine the National League pennant, Alou's pinch-hit single to lead off the ninth inning began a four-run rally that lifted the Giants to a 6-4 win over the Dodgers and into the World Series.
"Although he played for six different teams, Matty remained a part of the Giants family as a long-time employee and will be forever linked with his brothers -- Felipe and Jesus -- as the first all-brother Major League outfield," the Giants said in offering condolences to Alou's family.
Born in the Dominican Republic on Dec. 22, 1938, Alou was signed by the New York Giants in 1957, joining his older brother Felipe, who had been signed two years earlier. Younger brother Jesus was signed in 1958, at age 16.
Matty made his Major League debut near the end of the 1960 season, and played with Felipe through 1963, after which Felipe was traded to the Milwaukee Braves. The three brothers played together briefly, after Jesus reached the big leagues in 1963. Matty and Felipe played together again with the Yankees in 1973. The brothers combined to play in 47 Major League seasons.
Matty Alou was also the uncle of Felipe's son Moises, a longtime Major League outfielder, and former pitcher Mel Rojas.