Hardin attended Memphis State University to play baseball from 1961 to 1962. While at Memphis State, he turned down offers to go pro, and after only 14 college games, Hardin signed a contract with the New York Mets, which included a $10,000 bonus. Despite higher offers from other teams, Hardin picked the Mets, at the time a new expansion team with a lot of opportunities. Hardin spent three years in the Mets' minor league system before he drafted by the Baltimore Orioles in the 1965 minor league draft. In 1967, he was called up from the minor leagues to replace an injured Jim Palmer.
On May 10, 1969, in a relief appearance, Hardin hit a game-winning walk-off home run in the bottom of the ninth inning in Baltimore's Memorial Stadium. On July 27, 1969, Hardin starred in the Orioles' most dominant shut-out victory in their history, routing the Chicago White Sox, 17–0. Hardin took the win over Billy Wynne, allowing just two hits with five strikeouts and also hit a home run in the fourth inning off Gary Bell. He pitched a complete game shutout on May 26, 1970, against the Cleveland Indians, allowing only five singles in the game. Three weeks later, Hardin pitched ten innings surrendering only six hits with zero walks versus the Washington Senators. The Orioles prevailed 3–2 in 13 innings with Pete Richert earning the win with three relief innings. In Cleveland on August 6, 1970, Hardin threw a complete game five-hitter in the second game of a doubleheader against the Indians. Hardin helped himself with a two-run triple in the second inning and also picked up another RBI by drawing a bases-loaded walk in the eighth inning. As a member of the Atlanta Braves on June 28, 1972, he hit a 2-out solo home run in the 4th inning off the Padres' Fred Norman in San Diego Stadium.
While Hardin was with the Orioles, Palmer reported that some of the players did not like him very much. "But Brooks Robinson and Davey Leonhard and me, we think he's a decent guy if you get to know him, which most of the others didn't do." "Hardin really was an impressive pitcher before he hurt his shoulder," Palmer described him. "He had great control."

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