The collection is arranged into three series, Series 1: Original Work, Series 2: Correspondence and Personal Materials, and Series 3: Bound Publications.

Series 1: Original Work is subdivided into 5 subseries: 1.1 Editorial Cartoons by Subject are undated final-draft editoral cartoons organized by primary subject. They are then arranged alphabetically in the finding aid for ease of discoverability. Physically they are arranged by subject and by size. Oversized materials are housed separately from smaller materials. 1.2 Editorial Cartoons by Date are arranged chronologically. 1.3 Editorial Cartoon Drafts are drafts of Larsen's editorial cartoons, filed alphabetically by subject. 1.4 Other Original Work is cartoonist work from Larsen outside of his editorial cartoons, including RPI classwork, Carrier Toons, mock-ups, and sketches. They are arraned alphabetically and chronologically therein. 1.5 Other Print Works are published copies of Larsen's original works, including book jackets and magazine covers, work for municipal governments, flyers, RPI publications, and newspaper clippings. They are arranged alphabetically and chronologically therein.

Series 2: Correpsondence and Personal Materials contains the correspondence of Chick Larsen, as well as a few family photographs. This series is arranged alphabetically and then chronologically.

Series 3: Bound Publications contains bound materials such as conference programs, catalogs, and books. They are arranged alphabetically and then chronologically.