In the years after leaving football, especially, he became a force in his community -- helping at-risk children and those addicted to drugs and alcohol.
Police say Smith, 34, was shot to death, and his wife was shot and injured, after a crash.
"We are devastated and saddened by Will's tragic and preventable death due to a senseless act that will leave a lasting scar on our community forever," Saints owner Tom Benson and his wife, Gayle, said in a statement. "Will was more than an exceptional football player. He was a father, a husband, a son, a brother and teammate to so many and an inspiration to countless more."
Born in Queens and reared in Utica, New York, Smith attended Ohio State University, where he played on the Buckeyes' 2002 national championship team.
But it was a game two years later, in 2004, that then-Ohio State coach Jim Tressel said stood out to him, according to the Cleveland Plain Dealer
. It was in the runup to a disappointing appearance in the Fiesta Bowl after Ohio State had lost out on a chance to return to the championship game.
"That was not a glamorous Fiesta Bowl" The Plain Dealer quoted Tressel as saying. "But when we got there, Will stood up and said he didn't want to hear anything about not wanting to be there, and he didn't want to see anything but everybody working hard to win the game in front of us."
"He not only spoke that way, he practiced that way the whole time we (were) there," Tressel told the paper. "And he easily could have held something back to avoid injury since he was going into the NFL draft."
Later that year, the Saints made him the 18th pick in the draft. He went on to play his entire career, 10 seasons, with the Saints, including the 2010 squad that beat the Indianapolis Colts in the Super Bowl.
The 2006 Pro Bowler played 139 games for the Saints, starting in 120, and racked up 618 tackles, 67.5 sacks, 19 forced fumbles and seven recovered fumbles. He ranks fourth among the Saints' all-time sack leaders and is considered one of the franchise's great defensive players.
He was "a force on the football field, a team and locker room leader both on and off it as a defensive team captain," the team said in a statement after his death.
He suffered a knee injury during the 2013 preseason, and the Saints released him in 2014.
New England signed him, but he never took the field for the Patriots, who released him later that year.
In the years since leaving football, Smith continued charitable activities, including his foundation, Where There's A Will, There's A Way
. The organization mentors and provides support for at-risk children in Louisiana and upstate New York. He also sat on the advisory board of The Artists and Athletes Alliance
He also played a big role in Kingsley House
, as well as Bridge House and Grace House
, and according to the Saints, he had been hosting an annual Smith Family Christmas event for Kingsley House families since 2012.
The event, which was often held at the Saints practice facility, included a holiday meal, Christmas gifts from Santa Claus and a tour of the facility.
The Smiths hosted a celebrity waiter event for Bridge House and Grace House, which teach people who have become dependent on drugs or alcohol how to live sober and productively, the team said. Smith persuaded his teammates to serve as waiters for the event, even after he retired from football.
In addition, Smith sponsored a Utica event called "Evening With All-Stars," which honors the region's high school football stars.
His last public Facebook post
shows him at the United Nations on Wednesday, the same day the world body observed the International Day of Sport for Development and Peace
He wrote on his personal website
that he wanted to be an FBI agent after his football career.
A life not without controversy
Despite the raft of accolades on and off the field, Smith did have blemishes on both his personal and professional record.
In 2011, the NFL suspended him for two games without pay for violating the league's policy on performance-enhancing substances three years before, according to the league.
He was one of four players to test positive for the banned diuretic StarCaps in 2008, the league said. The NFL fined him an additional two game checks, according to the league
The following year, the league suspended him for four games after he and three other Saints were implicated in the franchise's "bountygate" scandal
The NFL later lifted the suspension.
According to the NFL's allegations, the Saints paid bonuses for targeting and injuring opposing teams' players between 2009 and 2011.
Off the field, police arrested Smith in 2010 and charged him with public intoxication and domestic abuse battery after he allegedly dragged his wife of three years, Raquel, by her hair outside a Lafayette, Louisiana, nightclub, according to The Times-Picayune
. He and his wife said it was a misunderstanding, the newspaper reported. Prosecutors dropped the charges at his wife's request after he completed community service and counseling requirements, the newspaper reported in 2012
In addition to his wife, he leaves behind three children -- William, Lisa Mya and Wynter Chase.
'Humble, caring selfless'
His death struck the sports community, and New Orleans, hard.
"The senseless acts of violence have to stop," New Orleans Mayor Mitch Landrieu said on Facebook
. "Traffic accidents should not lead to someone losing their life."
Players and coaches from throughout Smith's career also took to social media to express their condolences.
His former coach at Ohio State, Tressel, tweeted Sunday that Smith was a "humble, caring, selfless family man."
Former NFL running back Thomas Jones lamented Smith's death in a series of tweets Sunday.
"Will Smith was a great example of how most NFL players REALLY are and not how we are PORTRAYED!" Jones wrote in one post
. "A low key, quiet, hard working family man."
"This one," he wrote
, "hurts bad."