Arenas appeared in 80 games and averaged a career-high 29.3 points per game ranking fourth in the NBA in scoring (29.3 ppg) in his 3rd year. He was selected to his second consecutive NBA All-Star Game, but only after a spot opened up due to an injury. Gilbert started to call himself the “East Coast Assassin”. He ranked second in the NBA in three-point field goals made (199), third in minutes per game (42.3) and free throws made (655), fourth in steals per game (2.01), and 18th in assists per game (6.1) including being named Eastern Conference Player of the Week three times. He set an NBA record for points scored in a game by a player who played 30 or fewer minutes when he scored 46 points in 30 minutes vs. New York (2/25).

In the 2006 Playoffs, Arenas led the NBA in scoring during with 34.0 points per game in six games vs. Cleveland and including a career playoff-high 44 points at Cleveland. He was named to the All-NBA Third Team for the second consecutive year. In the summer, he was invited to try out and represent the United States in the USA Men’s Senior National Team program but was later cut from the team.