Baker, who was hired by the Tar Heels on January 10, will coach the Cowboys' defensive line.
"I appreciate what Brian gave to our program, even though he was here just a short amount of time," said UNC head coach Butch Davis in a statement.
"After accepting the UNC job, I turned down other offers to return to the NFL. While this was a difficult decision for me and my family, the Dallas Cowboys provided an opportunity I couldn't refuse," said Baker.
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