The collection features an impressive concentration of eighteenth and early nineteenth century portraits and history paintings by John Singleton Copley, Ralph Earl, Rembrandt Peale, Gilbert Stuart, Thomas Sully, John Trumbull, John Vanderlyn, and Benjamin West.

The core of the Museum's renowned Hudson River School collection (the finest of its kind) was formed by two major patrons of American artists who lived in Hartford—Daniel Wadsworth (1771-1848), a picaresque traveler, amateur artist and architect, and founder of the Wadsworth Atheneum; and Elizabeth Hart Jarvis Colt (1826-1905), widow of arms manufacturer Samuel Colt and the creator of a major private picture gallery during the Civil War Era. Wadsworth became one of the most important patrons of Thomas Cole, from whom he commissioned and acquired seven paintings; he later discovered and launched the career of the young Hartford artist Frederic Church. Wadsworth's private art collection formed the core of the Museum's American painting holdings. Later in the century, Elizabeth Colt worked with Frederic Church to form one of the finest private picture galleries in the country including works by Church, Albert Bierstadt, Sanford Gifford, and John Kensett. The collection of over 65 Hudson River landscapes includes thirteen Coles, eleven Churches, and five Bierstadts. The paintings are currently traveling as an exhibit in Europe (see Traveling Exhibitions).

Additional areas of concentration include the post-Civil War Era with paintings by William Merritt Chase, Thomas Dewing, Thomas Eakins, Winslow Homer, Eastman Johnson, Albert Pinkham Ryder, John Singer Sargent, and James McNeil Whistler. American impressionism is highlighted with paintings by Childe Hassam, Willard Metcalf, John Twachtman, and J. Alden Weir.

The early decades of the twentieth century are represented with extraordinary examples of Ash Can school artists John Sloan, George Bellows, and William Glackens; early Modernists including Stuart Davis, Arthur Dove, Marsden Hartley, Georgia O’Keeffe, and Florine Stettheimer; American Surrealists Joseph Cornell, Yves Tanguy, and George Marinko; and American Realists Maxfield Parrish, Norman Rockwell, and Andrew Wyeth.

The sculpture collection is equally distinguished with especially strong holdings in Neoclassical works by Edward Bartholomew, Horatio Greenough, Harriet Hosmer, and Hiram Powers; and major twentieth century works by Alexander Calder, Gaston Lachaise, Paul Manship, and Elie Nadelman.

The collection of works on paper, including watercolors, drawings, and prints, features works by many of the artists represented in the paintings collection, with strengths in the area of eighteenth-century portraiture and history paintings, nineteenth century landscape, and post-Civil War figurative works. Of particular note are the exceptional holdings in the area of American Modernist watercolor, including works by Charles Burchfield, Charles Demuth, Arthur Dove, Edward Hopper, and John Marin. In addition, the museum has a small but select group of American photographs, ranging from mid-nineteenth century daguerreotypes to early twentieth century silverpoint prints.