Harrison's agent, William Parise, said Harrison had a physical and met with coach Bruce Arians but the prospective deal broke down over money.
The 36-year-old Harrison played last year with Cincinnati, starting in 10 games and getting two sacks.
Harrison played his first nine NFL season with the Steelers before going to Cincinnati.
Cardinals fans remember him most for intercepting Kurt Warner's pass late in the first half of the 2009 Super Bowl and returning it 100 yards for a touchdown.
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