Thanks in large part to Crane's efforts, the broad and varied collections of Berkshire Museum include over 40,000 objects from virtually every continent—from important fine art and sculpture to natural science specimens and ancient artifacts.

[3][4] Crane purchased many of Berkshire Museum's first acquisitions, including a sizable group of paintings from the revered Hudson River School.

[5] The diverse collections also boast artifacts of ancient history and natural science: fossil collections, a 143-pound meteorite, an Egyptian mummy, shards of Babylonian cuneiform tablets, samplings of early Mediterranean jewelry, and representations of Berkshire ecosystems including local mammals, birds, reptiles, fish, insects, plants, and minerals.

The writing desk of Nathaniel Hawthorne and the musket believed to have belonged to Israel Bissell (a cohort of Paul Revere who made a midnight ride to Philadelphia to warn, "The British are coming!")

In the 1950s, the Berkshire Museum was the first to display the work of Norman Rockwell, as well as pieces by artists that challenged convention, such as Andy Warhol, Red Grooms, Robert Rauschenberg, Ellsworth Kelly, and Nancy Graves.

In the 21st-century, acquisitions have focused on artists with national and international reputations who have strong connections to the Berkshires: Gregory Crewdson, Peter Garfield, Morgan Bulkeley, Stephen Hannock, Tom Patti, and others.

In order to remain solvent, in July 2017, the Board of Directors at the Berkshire Museum announced a plan to sell the most significant portion of their art collection including two Norman Rockwell paintings, Blacksmith's Boy – Heel and Toe (Shaftsbury Blacksmith Shop) (1940) and Shuffleton's Barbershop (1950), which were given to the museum by Norman Rockwell himself.

[13] On November 1, 2017, before a packed courthouse, Superior Court Judge John A. Agostini heard arguments on both sides of the controversy centered on the right of the plaintiffs to sue.

[15] Judge Agostini, when ruling that the sale could proceed, wrote that the Attorney General’s four-month investigation “has uncovered no evidence of bad faith, no conflict of interest, no breach of loyalty, no express gift restrictions, and yielded unconvincing evidence of implied gift restrictions or a breach of reasonable care during a two-year decision-making process.”[14] The Superior Court deemed it “beyond objection” that the Museum’s “financial outlook is bleak.”[14] Nevertheless, the Massachusetts Appeals Court granted a temporary injunction to halt the sale that expired on December 11.