Before arriving at Alabama, Bryant was head football coach at University of Maryland, the University of Kentucky, and Texas A&M University.

Paul Bryant was the 11th of 12 children who were born to William Monroe and Ida Kilgore Bryant in Fordyce, Arkansas. His nickname stemmed from his having agreed to wrestle a captive bear during a theater promotion when he was 13 years old.

He attended Fordyce High School in Fordyce, Arkansas, where 6 ft 1 in (1.85 m) tall Bryant, who as an adult would eventually stand 6 ft 3 in (1.91 m), began playing on the school's football team as an eighth grader. During his senior season, the team, with Bryant playing offensive line and defensive end, won the 1930 Arkansas state football championship.

Bryant accepted a scholarship to play for the University of Alabama in 1931. Since he elected to leave high school before completing his diploma, Bryant had to enroll in a Tuscaloosa high school to finish his education during the fall semester while he practiced with the college team. Bryant played end for the Crimson Tide and was a participant on the school's 1934 National Championship team. Bryant was the self-described "other end" during his playing years with the team, playing opposite the big star, Don Hutson, who later became an NFL Hall-of-Famer. Bryant himself was second team All-SEC in 1934, and was third team all conference in both 1933 and 1935. Bryant played with a partially-broken leg in a 1935 game against Tennessee. Bryant pledged the Sigma Nu social fraternity, and as a senior, he married Mary Harmon.

Bryant was selected in the fourth round by the Brooklyn Dodgers in the 1936 NFL Draft, but never played professionally.

After graduating in 1936, Bryant took a coaching job at Union University in Jackson, Tennessee, but he left that position when offered an assistant coaching position under Frank Thomas at the University of Alabama. Over the next four years, the team compiled a 29–5–3 record. In 1940, he left Alabama to become an assistant at Vanderbilt University under Henry Russell Sanders. After the 1941 season, Bryant was offered the head coaching job at the University of Arkansas. However, following the bombing of Pearl Harbor, Bryant joined the United States Navy. He served off North Africa, seeing no combat action. However, his ship, the civilian merchantman SS Uruguay was rammed by another ship and ordered to be abandoned. Bryant disobeyed the order, saving the lives of his men. Two hundred others died. He was later granted an honorable discharge to train recruits and coach the North Carolina Navy Pre-Flight football team. One of the players he coached for the Navy was the future Pro Football Hall of Fame quarterback Otto Graham. While in the Navy, Bryant attained the rank of Lieutenant Commander.

In 1945, 32-year old Bryant met Washington Redskins owner George Marshall at a cocktail party hosted by the Chicago Tribune, and said he had turned down offers for assistant coaching positions at Alabama and Georgia Tech. Bryant told Marshall that he was intent on becoming a head coach. Marshall put him in contact with Harry Clifton "Curley" Byrd, the president and former football coach of the University of Maryland.

After meeting with Byrd the next day, Bryant received the job as head coach of the Maryland Terrapins. In his only season with at Maryland, Bryant led the team to a 6–2–1 record. However, Bryant and Byrd came into conflict. In the most prominent incident, while Bryant was on vacation, Byrd reinstated a player who had been suspended by Bryant for a violation of team rules. After the 1945 season, Bryant left Maryland to take over as head coach at the University of Kentucky.

Bryant coached at the University of Kentucky for eight seasons. Under Bryant, Kentucky made its first bowl appearance (1947) and won its first Southeastern Conference title (1950). The 1950 Kentucky team concluded its season with a victory over Bud Wilkinson's #1 ranked Oklahoma Sooners in the Sugar Bowl. The living players from the 1950 team were honored during halftime of a game during the 2005 season. Bryant also led Kentucky to appearances in the Great Lakes Bowl, Orange Bowl, and Cotton Bowl Classic. Kentucky's final AP poll rankings under Bryant included #11 in 1949, #7 in 1950, #15 in 1951, #20 in 1952 and #16 in 1953. The 1950 season was Kentucky's highest rank until it finished #6 in the final 1977 AP poll.

Bryant departed Kentucky after he and basketball coach Adolph Rupp had both completed successful seasons in their respective sports. Legend has it that, as a reward, Rupp was given a Cadillac automobile; Bryant was given a cigarette lighter. Bryant left Kentucky, furious that the university had not reprimanded Rupp for his players' roles in the college basketball point-shaving scandals of the early '50s. Kentucky was suspended from playing college basketball in 1953, and Rupp received no suspension. This led Bryant to conclude that basketball was #1 on the Kentucky campus and Bryant could not abide by that. Rumors also stating that Bryant left Kentucky after his ideas of integrating the team were rebuffed.