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The Manuscripts collection contains information covering numerous aspects and periods of Lyme history.

A collection of newspaper supplements on Lyme published by the Main Street News of Essex, Conn.

The Sylvia Daniels Harding (1911-1997) papers include her personal and many Harding, Ely, and Daniels family papers. Included are her own and her mother's diaries; photographs and vintage postcards of local sites and community life in late 19th and early 20th century Lyme — domestic life, farming, dairying, shad fishing, fur trapping, and the raw fur business, one-room schools, church, Grange, Sylvia's community work, organization memberships, and folk art "needle painting".

The Book collection contains books about Lyme, or on topics relevant to interpreting or contextualizing Lyme's history.

The Ely papers are the papers of three prominent physicians of Lyme from the Ely family: Dr. Josiah Griffin Ely, Sr. (1829-1887), Josiah Griffin Ely, Jr. (1857-1935), and Julian Griffin Ely (1894-1980).

Photographs by Winifred Webster of Hamburg Fair, farmer personalities, and landmark structures in Lyme.

The papers, correspondence, and genealogical research of William Beebe include more than two hundred fifty Lyme families from the 17th into the 20th century including his own Beebe and Royce families. His work includes many families in the northeast area of the town and often includes property boundary sketches.

The history and operational detail in photographic and text form of A Year at Tiffany Farms, 2002, documenting a full year on one of few dairy farms left in Connecticut at the time. The collection provides a unique look at the operations of a small Connecticut dairy farm and its struggles.

The Maps collection is made up of 19th and 20th-century maps of the Lyme, Conn. area and lower Connecticut River Valley.

The Artifact Collection holds a variety of small objects having historical significance for Lyme's cultural history and community life.