Tolbert was born in Amarillo, and was raised in Wichita Falls and Canyon. He attended various colleges, but never received a degree. He worked as a sports writer for the Lubbock Avalanche-Journal, the Wichita Falls Times Record News, and the Fort Worth Star-Telegram. He also wrote articles that were published in Collier's, Esquire, and the Saturday Evening Post. He served in the Marine Corps during World War II, and married Kathleen Hoover in December 1943. In 1946 he joined the Dallas Morning News, and became a regular columnist on Texas topics.

He was also a food connoisseur, wrote a history of chili con carne called A Bowl of Red, and ran Tolbert's chili restaurant in Dallas. In 1967 he founded, with Wick Fowler, the World Chili Championship held annually in Terlingua, Texas, which was later named for them.

He died of heart failure at age 71. His son, Frank X. Tolbert II, is an artist and chili chef. His daughter, Kathleen Tolbert Ryan, re-opened a Tolbert's Restaurant in May 2006 on Main Street in Grapevine, Texas. Another daughter was Bertha Theil Tolbert.

Fiction

• Bigamy Jones (1954)
• The Staked Plain (1987) with Tom Pilkington, Southern Methodist Univ. Press, ISBN 9780870742538.

Non-fiction

• An Informal History of Texas (1951)
• Neiman-Marcus, Texas (1953)
• The Day of San Jacinto (1959) Jenkins Publishing.
• Dick Dowling at Sabine Pass (1962)
• A Bowl of Red (1972) Doubleday, ISBN 9780385057639.
• Tolbert's Texas (1983) Doubleday, ISBN 0385085826, 9780385085823.
• Tolbert of Texas: the Man and His Work (1986) ed. by Evelyn Oppenheimer, TCU Press, ISBN 0875650686, 9780875650685.