As a college player, Smith was named Big East Player of the Year. He was a member of the University of Pittsburgh's highly touted five-man recruiting class considered the country's best. Along with power forward Jerome Lane, Charles Smith and the Pitt Basketball Team became a major force in college basketball, opening the 1987–88 season ranked No. 4 nationally and rising as high as No. 2. However, the Panthers never won a national championship during Smith's tenure.

He played for the US national team in the 1986 FIBA World Championship, that won the gold medal. and the 1988 Olympics which won a bronze medal.

After his college career, the 6'10", 230 lb power forward was selected 3rd overall in the 1988 NBA draft by the Philadelphia 76ers but immediately traded to the Los Angeles Clippers. After four years with the Clippers where he was among the team's top scorers and rebounders, he was traded to the New York Knicks with Doc Rivers and Bo Kimble for point guard Mark Jackson. Smith was expected to fill the hole at small forward left by Xavier McDaniel after the Knicks failed to re-sign him after their successful 1991–92 season, a role that Smith struggled in as he was primarily a power forward. As Smith's stats declined, he was traded to the San Antonio Spurs for J. R. Reid before retiring in 1997 due to severe injuries.

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