While still a WNBA player, she started coaching the Temple University Owls women's basketball team in 2000. In eight years at Temple, she led the program to six NCAA tournaments, three regular season conference championships, and four conference tournament titles.
On May 7, 2008, she was named head coach for women's basketball at the University of South Carolina. Staley built South Carolina from the ground up. In her first six seasons as head coach, she improved her program's record every year, winning the SEC in 2013–2014. In late 2014 her team achieved the program's first #1 ranking, making her only the second individual to both play on and coach a #1 ranked team. Staley has gone on to lead South Carolina to six SEC regular season championships, six SEC tournament championships, eight Sweet Sixteens, four Final Fours, and two NCAA Women's Basketball National Championships.
On April 2, 2020, Staley became the first person to win the Naismith Award as both a player and a coach. She also won the other three major National Coach of the Year awards after she led her team to a 32 win season and a final ranking of #1 in both major polls.

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