In 2001, he had the best year of his college career. He started the season by being voted as the team captain, and in the season opener he recorded seven tackles and one tackle for a loss against San Jose State. Against Kansas State, he had a game-high 13 tackles, three tackles for a loss, and one forced fumble. Polamalu continued his dominance against Stanford, making a game-high 10 stops, one tackle for a loss, and his first blocked punt of the season. In the next game against Washington he had a game-high 13 tackles, two tackles for a loss, an interception that he returned for a 22-yard touchdown. Throughout the next four games, Polamalu continued to have the most tackles in each game. He had a streak of six games in a row and eight total in the season where he led both teams in tackles. Against Oregon State, he accumulated a game-high 11 tackles, two tackles for a loss, two pass deflections, one forced fumble, and a blocked punt that USC recovered. His streak ended against California, when he had four tackles, but made a game-deciding play with an interception that he returned for a 58-yard touchdown. The next week, the Trojans played their rival, UCLA. Polamalu had two tackles but made key plays when he blocked a punt and made an interception that set up key field goals for USC. He won his first PAC-10 Defensive Player of the Week. USC went on to the Las Vegas Bowl against Utah and Polamalu made a career-high 20 tackles, and three tackles for a loss. He finished his junior campaign with a team-high 118 tackles, 13 tackles for a loss, one sack, three interceptions, two forced fumbles, one fumble recovery, three blocked punts, and two touchdowns. Polamalu won USC's MVP award and was voted a first-team All-American by Football Writers and College and Pro Football News Weekly. The Associated Press voted him second-team All-American.