Blair died Thursday night at Sinai Hospital of Baltimore, according to a hospital spokeswoman.
Blair's wife, Gloria, told The Baltimore Sun, that Blair played a round of golf with friends Thursday morning and later lost consciousness at a celebrity bowling tournament in Pikesville.
"Paul was honestly too tired, but he never says no," Gloria Blair told the newspaper. "During a practice round, he threw two or three balls, then sat down and told a friend, 'I feel funny' and kind of collapsed. He lost consciousness and they called 911 and the ambulance took him to (Sinai), but the doctors there told me they never got a pulse."
A member of the Orioles Hall of Fame, the popular Blair patrolled the outfield from 1964-76, playing key parts when Baltimore won its first two World Series crowns in 1966 and 1970. He won two more titles with the New York Yankees in 1977 and 1978 and also played for Cincinnati.
In an era before highlight reels were a daily staple on TV, Blair frequently made catches that became the talk of baseball. Thin and quick, he played with a flair—at the end of an inning, he would tuck his glove up against his chest for a regal trot back to the dugout.
"He played very shallow.
"When you talk about the greatest defensive center fielders, he was right in the mix," Buford said. "With me in left and Frank Robinson in right, we played toward the lines and gave him a lot of room. He could really go get it."
In 17 seasons in the majors, he hit .250 with 134 home runs, 620 RBIs and 171 stolen bases. Blair appeared in six World Series, two All-Star games and won Gold Gloves in 1967 and 1969-75.
In the 1966 World Series, Blair homered for the only run in Baltimore's Game 3 victory over Los Angeles.
The underdog Orioles completed an unlikely sweep the next day, with Blair jumping high above the fence at Memorial Stadium to snare Jim Lefebvre's bid for a tying home run in the eighth inning. It was a timely grab, too—Blair had just been inserted in the game as a defensive replacement.
Blair caught a routine fly by Lou Johnson with two runners on base for the final out in a 1-0 victory in Game 4, and leaped high in the air after the clinching grab to begin Baltimore's celebration.
Blair led the Orioles in the 1970 World Series with a .474 average in Baltimore's five-game victory over Cincinnati. That year, he hit three home runs and had six RBIs in a game against the Chicago White Sox.
Beaned by a pitch in late May that season, Blair came back from the injury to boost the Birds. Ever mindful of being hit in the face, he would shield his face at first base when retreating to the bag on pickoff throws.
"It affected his hitting a little bit after that, but not his fielding," Buford said.
Inducted into the Orioles Hall of Fame in 1984, Blair coached Fordham in 1983 and at Coppin State from 1998-2002. He had a heart attack in December 2009.
Blair played baseball and basketball and ran track at Manual Arts High School in Los Angeles.
Blair was originally drafted by the New York Mets and spent one season in their minor league system. The Orioles drafted him from the Mets in late 1962.
He fit neatly into a team built on strong defense—led by third baseman Brooks Robinson—and pitching, and Baltimore reached the World Series four times in six years. He was surrounded by stars, yet a picture or drawing of Blair often made the cover of the Orioles' game programs.
Friendly in the clubhouse, he was called "Motormouth" for his constant banter.
"He'd be talking about something, and maybe you'd get two words in, and then he'd be off starting another conversation," Buford recalled.
AP Baseball Writer Ben Walker contributed to this report.