On April 24, 2001, Leonard Little agreed to a one-year tender offer of $512,000, the minimum level for a restricted free agent. That season, he changed his jersey number to 91 and was a pass-rush specialist for the NFC champion Rams. Little would enter games in passing situations in place of starting left defensive end Chidi Ahanotu.
In that role, Little led the Rams with 14.5 sacks, 3rd in the NFL. Little had nine tackles (five solo), three QB pressures, and one sack in Super Bowl XXXVI. On the first play of the New England Patriot game-winning drive Little brushed the ball but could not dislodge it from Tom Brady, who kept the drive alive by completing a short pass.