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James attended St. Vincent–St. Mary High School in Akron, where he became a starter during his freshman year for the Fighting Irish. He averaged 21 points and 6.2 rebounds, and led the team to a 23–1 record, en route to the Division III state title. Keith Dambrot, now head coach at the University of Akron, was the head coach at St. Vincent–St. Mary. Coach Dambrot started working with James doing $1 clinics at a local recreation center.[6] In his sophomore year, James averaged 25.2 points, 7.2 rebounds, 5.8 assists and 3.8 steals.[6] He led the team to a 26–1 record and a Division III state title for the second straight season.[33] He was the first sophomore to be named Ohio's "Mr. Basketball" and became the first sophomore ever selected to the USA Today All-USA First Team.[33]

In James' junior year his stats improved again. He averaged 29.0 points, 8.3 rebounds, 5.7 assists and 3.3 steals and was again named Mr. Basketball of Ohio.[33] He earned a spot on the All-USA First Team, and was named the 2001–2002 boys' basketball Gatorade National Player of the Year. It was at this time that his nickname "King James" became a household staple in Ohio.

James appeared in SLAM Magazine, which began his nationwide exposure. The St. Vincent–St. Mary basketball team did not defend its state title when increased enrollment forced the team to move up to the more challenging Division II (Ohio high school basketball has four divisions based on annual enrollment figures) and lost to Roger Bacon High School (Cincinnati). James considered declaring for the 2002 draft after the season ended by petitioning for an adjustment to the NBA's draft eligibility rules, which at the time required prospective players to have at least completed high school.[34] The petition was unsuccessful, but it ensured him an unprecedented level of nation-wide attention as he entered his senior year. By then, James had already appeared on the covers of Sports Illustrated and ESPN The Magazine. His popularity forced his team to move their practices from the school gym to the nearby James A. Rhodes Arena at the University of Akron. NBA stars such as Shaquille O'Neal attended the games, and a few of James' high school games were even televised nationally on ESPN2 and regionally on pay-per-view.

In 2003, James' mother, Gloria James, got approval of a loan to buy a Hummer H2 for her son's 18th birthday.[35] The bank took her son's future earning power into consideration, prompting an investigation by the Ohio High School Athletic Association (OHSAA).[35] Under the OHSAA guidelines, no amateur may accept any gift valued over $100 as a reward for athletic performance.[36] When James later accepted two throwback jerseys of Wes Unseld and Gale Sayers worth $845 from NEXT, an urban clothing store in Shaker Square, in exchange for his posing for pictures to be displayed on the store's walls, OHSAA stripped him of his eligibility.[36] James appealed and a judge blocked the ruling, reducing the penalty to a two-game suspension and allowing him to play the remainder of the season. James' team was forced to forfeit one of their wins as a result.[37] That forfeit was the team's only official loss that season.

Despite the distractions, the Irish won a third state title, with James averaging 31.6 points, 9.6 rebounds, 4.6 assists and 3.4 steals on the season.[33] James was named to the All-USA First Team for an unprecedented third time, and was selected as Mr. Basketball of Ohio for the third year in a row.[33] He earned MVP honors at the McDonald's All-American Game, the EA Sports Roundball Classic, and the Jordan Capital Classic.[citation needed] Although it was a foregone conclusion, by participating in more than two high school all-star events, James officially lost his NCAA eligibility.[38] James finished his high school career with 2,657 points, 892 rebounds and 523 assists.[33]