Transition metal dichalcogenides (TMDs), with superior mechanical and electrical conductivity, are one of the most promising two-dimensional materials for creating a generation of intelligent and flexible electronic devices. However, due to the high van der Waals and electrostatic attraction, TMD nanomaterials tend to aggregate in dispersants to achieve a stable state, thus severely limiting their further applications. Surface chemical modification is a common strategy for improving the dispersity of TMD nanomaterials; however, there are still constraints such as limited functionalization methods, low grafting rate, and difficult practice application. Thus, it is challenging to develop innovative surface modification systems. Herein, we covalently modify an olefin molecule on surface-inert MoS 2 , and the modified MoS 2 can be used as not only a catalyst for hydrogel polymerization, but also a cross-linker in the hydrogel network. Specifically, allyl is covalently grafted onto chemically exfoliated MoS 2 , and this modified MoS 2 can be uniformly dispersed in polar solvents (such as acetone, N , N -dimethylformamide, and ethanol), remaining stable for more than 2 weeks. The allyl-modified MoS 2 can catalyze the polymerization of polyacrylamide hydrogel and then integrate in the network, which increases the tensile strength of the composite hydrogel. The flexible sensor based on the composite hydrogel exhibits an ideal operating range of 600% and a quick response time of 150 ms. At the same time, the flexible device can also track the massive axial stretching movements of human joints, making it a reliable option for the next wave of wearable sensing technology.