Charlot collected and studied work that inspired him, including 18th and 19th century European prints, especially those of Honoré Daumier and the 19th century popular prints from the French town of Épinal, known collectively as “images d’Épinal.” In Mexico he collected the penny sheets of José Guadalupe Posada and built an outstanding collection. A selection of the latter is shown in the exhibition catalogue José Guadalupe Posada: My Mexico (University of Hawai‘i Art Gallery, 2001). The Posada Collection is so extensive that there is a separate guide listing all of the works.

The holdings include Pacific ethnographic art that Charlot acquired. In 2005, the collection was given an important gift of 19th century Mexican folk art and pre-Hispanic pots once belonging to Charlot’s maternal grandfather.

Charlot collected or was given art by artists with whom he worked or about whom he wrote. These include Mexican artists such as Xavier Guerrero, Leopoldo Méndez, Pablo O’Higgins, José Clemente Orozco, Diego Rivera, David Alfaro Siqueiros, and Alfredo Zalce; the Guatemalan Carlos Mérida; and internationally known photographers such as Tina Modotti and Edward Weston. Among the American artists are Louis Eilshemius, Lowell Houser, Henrietta Shore, Dorothea Tanning, and numerous artists from Hawai‘i.