Since LeBron opened the I Promise school in his hometown of Akron, Ohio, more than 16,000 people have signed the Care2 petition, which asks President Trump to get rid of DeVos in favor of the four-time National Basketball Association champ.
DeVos, who has been United States secretary of education since 2017, was described in the document as "a scandal-ridden Republican donor who shows an inexcusable dislike for public education".
James celebrated the opening of his "I Promise" public elementary school in his hometown of Akron, Ohio late in July - which will serving around 300 at-risk children and their families - providing them with free lunch, textbooks, classes, tutoring, and free bicycles.
Who would you rather?
President Trump with his secretary of education, Betsy DeVos, at the White House. Many critics argue that she is unqualified for the position and speak negatively of her wealth.
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Betsy DeVos was hired without ever setting foot in a public school - and she's taken every opportunity to work against the interests of the children, teachers, and families she has pledged to serve.
The petition has more than 5,000 supporters and is nearing its goal of 6,000 as of Wednesday afternoon.
James chose to open a traditional public school, not a charter school. He made Lebron look smart, which isn't easy to do. I like Mike!' Trump tweeted last Friday.
The U.S. Secretary of Education is appointed by the president and confirmed by the Senate.
'At least unlike Betsy DeVos, LeBron James supports education, ' Miranda Yaver hit back.
Last month, James gave an interview to CNN's Don Lemon in which he slammed Trump's policy, saying that was using sport to divide America along racial lines.