Due to the population explosion of the 21st century, nearly one billion people are over 64 years of age and bone fracture is one of the most frequent problems facing both sexes because of osteoporosis. However, difficulty in enhancing bone regeneration to repair bone fracture poses challenges and thus, a two-dimensional monolayer material (i.e. tungsten disulfide (WS2)) could be one of the candidates offering a possible solution to the problem. Here, we prepare high-quality monolayer WS2 thin sheets in a large quantity with the assistance of extracted chlorophyll molecules, the natural pigment used in photosynthesis, via a liquid-phase exfoliation method. Then, the exfoliated WS2 sheets were mixed with polycaprolactone (PCL)/calcium silicate (CS) to form a biocompatible WS2-based composite. The in vivo experiments show that the bone regeneration of the WS2-based composite was 120% superior to commercially available mineral trioxide aggregate (MTA) bone cement. Moreover, the mechanical properties of the WS2-based composite exhibited ~300% enhancement over PCL/CS, which is one of the most commonly used bone regeneration materials. Our findings highlight the prospects for the composite of WS2 towards the improvement of bone regeneration applications.