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The materials comprising the Collins papers range in date from the 1940s to the 1980s, with concentrations in Collins' terms as Governor and materials related to his 1968 unsuccessful Senatorial campaign. The collection consists of 344 manuscript boxes, approximately 200 linear feet of papers which include and are not limited to correspondence files, working papers, reports, campaign research, memoranda and speeches. The collection also includes approximately 35 scrapbooks, memorabilia, and an extensive amount of pictures. Film and recordings from the collection were transferred to the State Library and Archives of Florida for preservation.

This collection contains research materials used by Martin Dyckman for his 2006 book about former Governor Leroy Collins titled Floridian of His Century. Research materials include speeches from Leroy Collins before he became governor; an interview transcript with Premier Khrushchev during Collins' trip to the Soviet Union; newspaper columns written by Collins for the St. Peterburg Times and transcripts and audio recordings of interviews conducted by Dyckman.

The Thomas LeRoy Collins Papers, 1903-1991, largely document this Florida statesman's post-Gubernatorial career (1961-1991). While these materials are predominantly from this period, there are also files from his earlier years as Florida Representative, Florida Senator, and Florida Governor.