The USA Today selected Will Smith as one of its All-American picks his senior year at Thomas R. Proctor High School where he excelled as a Defensive End. The Prep Football Report ranked him the best defensive line prospect in New York State. He had 20 sacks during his senior season alone, and was named Mohawk Valley Player of the Year. As a result, Ohio State University offered Smith a full scholarship to play for the Buckeyes.

In Columbus, Smith got even better. As a freshman, he was named one of the Outstanding First-Year Defensive Players after having three sacks. His junior year accomplishments earned him an All-Big 10 Second Team spot as he was an integral part of a 14-0 Buckeye team that won the National Championship.

As a senior, Smith exploded to become one of Ohio State's best defensive products. Named a captain on the squad for his senior year, Smith committed 10.5 sacks bringing his career total to 23 - fifth in the school's history. On his way to earning an All-Big 10 Conference team spot, Big-10 Defensive Player of the Year honors and being named Defensive Lineman of the Year, Smith had 49 total tackles, 30 of which were solo. Smith was named a finalist for the Hendrick's Award, given to the nation's top Defensive End.

In 2004, the New Orleans Saints of the National football League drafted Smith in the first round, 18th overall.

A member of the Pro Football Weekly All-Rookie Team in 2004, Smith's freshman campaign saw him make 7.5 sacks and 6 forced fumbles. In his sophomore season, Smith had 85 total tackles, 66 of which were solo and 8.5 sacks which was eighth in the National Football League in 2005. Added to those terrific numbers were two forced fumbles, one fumble recovery and six pass deflections.

During that 2005 season, Smith set the New Orleans Saints' record for a Defensive End when he caused a fumble in five consecutive games.

Named Defensive Captain of the New Orleans Saints at the start of the 2006 season, Smith had 52 tackles and 10.5 sacks, for a loss of 80 yards. He had three forced fumbles and three pass deflections and as a result was named as a starter on the 2006 Pro Bowl, his first appearance on the team.