Series I: Correspondence is arranged chronologically by type of correspondence, including general, family, correspondence from a specific person, and correspondence on a single subject.

Series I: Correspondence contains a wide array of correspondents and recipients. General correspondence contains a wide range of subjects, though Margaret Sage stands out as a frequent author and recipient. Family correspondence contains letters to and from Gould family members, particularly her brother Frank Gould. Correspondence regarding Jay Gould mainly contains reminiscences of Jay Gould from friends and relations in response to Helen's efforts to gather information about her father. Correspondence regarding Joseph Wheeler contains letters from the congressman regarding Helen's Congressional recommendation. Correspondence regarding the Y.M.C.A. and soldiers contain both official letters from administrators in the Y.M.C.A. organizations as well as personal letters from individual soldiers. Finally, correspondence regarding the donation of artwork contains a series of letters to and from Helen regarding her personal donation of artwork to various institutions.

In general, the earliest correspondence contains more intimate letters sent to and from Helen and her parents and friends, particularly Margaret Sage. Later correspondence is more formal, mostly relating Helen Miller Gould Shepard's philanthropic and religious work.

Series II: Writings by Helen Miller Gould Shepard is arranged by type and then chronologically.

Series II: Writings by Helen Miller Gould Shepard contains both personal and published documents created by Helen Miller Gould Shepard including sketchbooks, school composition notebooks, a travel diary, and copies of religious tracts published by Helen. Sketchbooks include both tracings and original sketches by Helen as a young girl. The six notebooks in the series are Helen's school notebooks from Miss Jaudon's School in New York City on various humanities subjects, some of which are written in French. The travel diary chronicles her trip to Europe and Egypt, traveling on the Gould yacht "Atlanta" (Oct. 1877-Feb. 1888).

Series III: Ephemera is arranged by type and then chronologically.

Series III: Ephemera makes up the largest series in this collection. Most items in this series pertain to Helen Miller Gould Shepard's philanthropic activities, including her work for war relief, religious groups, and for institutions such as New York University. A large portion of this series is comprised of certificates of membership and of gratitude for charitable works.

Series IV: Scrapbooks contains two bound and three unbound scrapbooks. Except for the scrapbook containing translated copies of "Passages to Memorize" leaflets, the remaining three scrapbooks are comprised of newspaper clippings regarding a specific topic or event and are arranged chronologically. Notable in this series in a bound volume which was given as a gift from Congressman Joseph Wheeler and contains clippings regarding Helen Miller Gould Shepard's Congressional commendation following her $100,000 donation to the federal government of the United States.

Series V: Published Material contains published materials not created by Helen Miller Gould Shepard. Notable in this series are copies of the Woody Crest Monthly leaflets, published by the children and caretakers at Helen Miller Shepard Gould's home for physically handicapped children.

Series VI: Visual Material contains photographs, photographic negatives, and photostat copies of church documents and certificates of Helen Miller Gould Shepard's wedding. Two photographs depict Jay Gould as a young man and in adulthood and one depicts Helen's mother, Helen Day Miller. The negatives show Helen Miller Gould with unidentified family members.