Octopus sinensis, commonly known as octopus, is an important economic cephalopod along the coast of China. With many favorable breeding characteristics such as high feed conversion rate, rapid growth and short breeding cycle, it is a new farming variety with great development potential. Bivalves are commonly used in O. sinensis culturing. Understanding the predation behavior and feeding selectivity of O. sinensis on bivalves is of great significance for screening suitable bivalves, improving feeding technology and perfecting breeding processes. In this paper, four kinds of bivalve bait, Chlamys farreri, Crassostrea gigas, Scapharca broughtonii and Ruditapes philippinarum were selected. The predation behavior of O. sinensis was recorded by underwater camera, and the feeding rate, amount and proportion of O. sinensis to various bivalves were statistically analyzed. The results showed that O. sinensis exhibited similar predatory behaviors among the four bivalve species, including attack, capture, shell opening, feeding and shell abandoning. O. sinensis had the highest feeding rate and intake of C. farreri, which were significantly higher than the other three bivalves (P < 0.05), and the lowest on C. gigas, which might be related to the difficulty levels in opening bivalve shells. The results indicated that C. farreri was a suitable prey for O. sinensis, and the ratio of C. farreri could be appropriately increased in octopus culturing to promote the growth and development.