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According to a Hollywood Reporter news item, James Stewart was originally set to star in the film. News items in Los Angeles newspapers note that Wallace Beery accidentally shot himself in the leg with a blank from his gun on September 13, 1937, during one of the film's action sequences. He was then taken to Cedars of Lebanon Hospital and, according to the news reports, was unable to work for about two weeks. An unidentified review of the film dated February 1938, contained in the AMPAS Library file on the film, mentioned that the character of "Trigger" Bill was a composite of actual Old West outlaws James H. "Dog" Kelley, Blinky Jones and Dr. John W. "Doc" Holliday.
Large segments of the film were shot on location in Zion National Park and Kanab, Utah. A January 17, 1938 news item in Hollywood Reporter noted that the success of this picture was signaling a change for M-G-M to produce more "outdoor" pictures. This was the first major film role for actor Dennis O'Keefe, whose real name was Edward Vance Flanagan and who had previously acted in numerous bit parts at M-G-M and other studios under the name Edward James Flanagan, or Bud Flanagan. According to a news item in Motion Picture Herald, Flanagan was henceforth going to be known as "Larry Doyle," but the actor apparently never used the name Doyle in a film, and Bad Man of Brimstone marked the first time he used the name "Dennis O'Keefe." Modern sources indicate that he was brought to the attention of M-G-M executives by Clark Gable, who noticed the young actor in a bit part in his 1937 picture, Saratoga. O'Keefe starred in several light comedy films for M-G-M before going to other studios. Wallace and Noah Beery were brothers. According to modern sources, this film marked the first time they appeared together since 1916.