The Wildcats announced Friday that Murray will join Kevin Sumlin's staff as running backs coach.
"DeMarco brings a wealth of knowledge and experience to our running back room," Sumlin said in a statement. "That, with his attention to detail, passion for the game and passion for impacting others will make him a great addition. Our entire staff is excited for him to join our organization."
Murray retired from the NFL in July, concluding a seven-year career that saw him lead the AFC in rushing in 2016 with the Titans. Tennessee released him in March.
Murray, who turns 31 next month, ran for 7,174 yards and 49 touchdowns in his career, averaging 4.5 yards per carry. He also had 307 receptions for 2,165 yards and six scores.
Murray starred in college at Oklahoma, where he was recruited by Sumlin, a Sooners assistant.
"I'm humbled to have the opportunity to start my coaching career with Coach Sumlin and the University of Arizona," Murray said. "My family and I are thrilled to become a part of the Tucson community, and I can't wait to get started. Bear Down!"