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 7 tackles and 1 tackle for a loss against San Jose State. Against Kansas State, he had a game-high 13 tackles, 3 tackles for a loss, and 1 forced fumble. Polamalu continued his dominance against Stanford, making a game-high 10 stops, 1 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, 2 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 6 games in a row and 8 total in the season where he led both teams in tackles. Against Oregon State, he accumulated a game-high 11 tackles, 2 for a loss, 2 pass deflections, 1 forced fumble, and a blocked punt that USC recovered. His streak ended against California, when he had 4 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 2 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 then went on to the Las Vegas Bowl against Utah and Polamalu made a career-high 20 tackles, and 3 tackles for a loss. He finished his junior campaign with a team-high 118 tackles, 13 tackles for a loss, 1 sack, 3 interceptions, 2 forced fumbles, 1 fumble recovery, 3 blocked punts, and 2 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.