Abstract: Crab shells are an important feedstock for chitin production. However, their highly compact structure significantly limits their use for the production of chitin under mild conditions. Here, a green and efficient approach using a natural deep eutectic solvent (NADES) to produce chitin from crab shells was developed. Its effectiveness in isolating chitin was investigated. The results showed that most proteins and minerals were removed from crab shells and the relative crystallinity of the isolated chitin reached 76%. The quality of the obtained chitin was comparable to chitin isolated by the acid–alkali method. This is the first report on a green method for efficient chitin production from crab shells. This study is expected to open new avenues for green and efficient production of chitin from crab shells.