Chalicotherium, like many members of Perissodactyla, was adapted to browsing, though uniquely adapted to do so among its ungulate relatives. Its arms were long and heavily clawed, allowing them to walk on their knuckles only. The arms were used to reach for high branches and bring them close to its short-faced head to strip them clean of leaves. The horse-like head itself shows adaptation to a diet of soft vegetation, since, as the animal reached sexual maturity, the incisors and upper canines were shed, suggesting that its muscular lips and the resulting gum pads were enough to crop fodder which was then processed by squarish, low-crowned molars.
Callosities on the ischium imply that these animals would sit on their haunches for extended periods of time, probably while feeding. Pad-supporting bony growth on the dorsal side of the manual phalanges is interpreted as evidence of knuckle-walking, which would probably be useful to avoid wearing down the claws, preserving them for use either as a forage-collecting rake or as a formidable defensive weapon.
All of these characteristics show some convergence with the unrelated ground sloths, gorillas and giant pandas.