Looney was drafted in the first round (twelfth overall) of the 1964 NFL Draft by the New York Giants. He was also selected in the sixth round of the 1964 AFL Draft by the Kansas City Chiefs, but chose to play in the NFL instead. He was with the Giants just 25 days before they traded him along with offensive lineman Lou Kirouac to the Baltimore Colts for wide receiver R.C. Owens and safety Andy Nelson during training camp on August 24, 1964. As a member of the Giants, Looney racked up a number of fines for violating team rules.