Born in West Virginia, Frank was known as a resident of Indianapolis, Indiana. Before turning to stock car racing, he had a varied athletic background: he served in the United States Marine Corps and competed as a Golden Gloves boxer. He began his motorsports career on motorcycles before progressing through sprint cars and midget cars, gaining broad experience on American oval circuits.
Frank made 38 starts in the 47-event 1956 NASCAR Convertible Series, one of the most active debut campaigns in that series. He made his NASCAR Grand National Division debut on October 28, 1956, in the Old Dominion 400 at Martinsville, Virginia, driving Lonnie Fish's No. 76 Chevrolet. He finished 38th after losing oil pressure on lap 77.
In 1957, Frank spent most of his time in the Convertible Series, competing in all but one race while also making four Grand National starts in Fish's No. 76 Chevrolet. His best finish of that year was 13th at Langhorne Speedway. During the 1958 NASCAR Grand National season, Frank competed in 11 events, recording a third-place finish in the Nashville 200 along with one top-five and four top-tens. Over the following seasons, Frank continued to make appearances in both Grand National and Convertible competition with modest results.
The defining moment of Frank's career came at the 1962 Southern 500 at Darlington Raceway. He qualified tenth for the race and went on to lead 85 laps, ultimately lapping the entire field. He finished the race on two blown tires. Junior Johnson initially received the checkered flag and was declared the winner.
However, car owner and pit chief Ratus Walters immediately challenged the outcome. A review by officials found that scorers had missed one of Frank's laps during the race. Three hours after the finish, NASCAR reversed the result and declared Frank the winner. The car he drove to victory carried the No. 66 — as of 2019, Frank remains the only driver to have won a NASCAR Cup-level race using that number.
Frank continued racing in the Grand National Division through the early and mid-1960s. In 1966, he decided to retire from competitive racing. Following his motorsports career, Frank opened Larry Frank's Auto Body Shop in Greenville, South Carolina, operating the business alongside his wife Margaret.
In 2009, Frank was diagnosed with lymphoma. He died on January 5, 2010, at his home in Greenville, South Carolina, at the age of 80.
Larry Frank occupies a small but distinct place in NASCAR history. His 1962 Southern 500 victory — reversed hours after the race ended following a scoring dispute — stands as one of the sport's more unusual championship corrections. The exclusivity of the No. 66 on a winning car, his path from motorcycles and midget cars through the Convertible Series to the Grand National division, and the dramatic nature of his biggest win ensure that Frank is remembered as a genuine, if undersung, figure of NASCAR's early era.