Born in Mobile, Alabama, Samuels attended Shaw High School in Mobile. Samuels was a basketball player in high school, but was lured to the football field after seeing most of his childhood friends join the Shaw team.
Samuels made his AFL debut in 1994 with the Tampa Bay Storm racking up 247 receptions through the 2000 season for over 3100 yards (3120 yards) in his first tenure with the Storm.
In 2001, Samuels left the Storm and played the season with the New Jersey Gladiators, catching 65 passes (a career high at the time) for 742 yards, just short of his 844-yard career high receiving season he recorded the year before with Tampa Bay.
After a single season in New Jersey, Samuels returned to Tampa, where he finished his playing career. From 2003-2007, Samuels notched 1,000+ yards receiving in 4 of 5 seasons, including back-to-back-to-back 1,100 yard+ seasons in 2005, 2006, and 2007. Was named MVP and Ironman of ArenaBowl XVII.
In 2007, after 5 losses to begin the season, Samuels was again named to the AFL's All-Ironman Team after leading the Storm to a #3 seed in the playoffs. 100+ catches, 1000+ yards, and 100+ TDs also helped Samuels earn the honor.
On June 15, 2008, Samuels became the first receiver in AFL history to record 1,000 career receptions. 
On August 10, 2013, Samuels was inducted into the AFL Hall of Fame.
In 2002 and 2003, he was an assistant coach and wide receivers coach at Central High School in Brooksville, Florida.
He was the offensive coordinator and receivers coach for the Wharton High School Wildcats during the 2005 and 2006 seasons.
In 2011, Samuels was named the offensive coordinator of the Storm, working with one of his former coaches, Dave Ewart.
Ewart was fired in early August 2013, and on September 5, 2013, Samuels was promoted to head coach of the Storm. Samuels and the Storm mutually agreed to part ways in August 2016.
His brother, Chris Samuels, was a 6-time Pro-Bowler in the National Football League
Lawrence is married to wife Kelli. They have two daughters.