The Margaret Storrs Grierson Papers contain materials related to Mrs. Grierson's career at Smith College as student, professor, college archivist and one of the founders and first director of the Sophia Smith Collection. In addition, there are her historic writings on the Storrs, Cooper, Rankin, Barnes and other related families and documents related to this work. There are biographical items, correspondence (especially with Nina E. Browne and with family members), diaries, financial records, passports, manuscripts and publications. Also included are photographs of the families as well as correspondence in relationship to Grierson's companion, Marine Leland.

The family papers are a mixture of documents (usually arranged under an individual or family name) and may contain a mixture of materials: historic documents and letters, photographs, printed materials and correspondence that spans from ca. 1800 to 1997. The files are essentially as Mrs. Grierson arranged them; in addition, the files contain correspondence by Mrs. Grierson and to her in her pursuit of documentation on particular family members. Also in the files are notations by Mrs. Grierson on the disposition of some historic documents that were once part of files but were placed in historic archives she deemed a more appropriate location for them to reside.