The collection consists primarily of records generated or accumulated during the educational and political (1949-1954) careers of Guilford M. Wiley, Sr. Those materials include correspondence (1931-1933; 1945-1954), scattered issues of the La Crosse Central High Tribune (1922; 1928), miscellaneous materials (circa 1938-1954), materials from the National Council of Presbyterian Men (1943-1954), and loose newspaper clippings grouped by topic (1939-1954). Many of the newspaper clippings pertain to information about the La Crosse School District, although other topics are covered as well.

Materials relating to other members of the Wiley family include a folder of family history and lineage of both the Wiley and Arnold families; photographs of Guilford M. Wiley, Sr. as a young man, photographs and a photo album of him and his wife Beulah (1944-1954), photographs of Wiley relatives, and an additional set of scanned photographs on a compact disk. In addtion, there are some materials which relate to Beulah Arnold Wiley, these include a diary (1972), a scrapbook from her time at Rockford (Illinois) College (1907-1908), and a scrapbook of her La Crosse friends (1942-1972). Lastly, there are some materials relating to Mary Esther Wiley Runnestrand: one photograph (ca. 1970s) and a teacher evaluation (1973).

Other materials include twenty photographic postcards depicting the evangelist Reverend Billy Sunday (1908), an indexed newspaper clipping scrapbook (1938-1939) containing articles pertaining to the La Crosse public schools.