Self-remodeling material can change their physical properties based on mechanical environment. Recently, mechanically controlled polymerization using mechanoredox catalyst enabled composite materials to undergo a permanent structural change, thereby enhancing their mechanical strength. However, a significant delay in material's response was observed due to the sluggish activation of the bulk catalyst for polymerization. Herein, we report a fast, mechanically controlled radical polymerization of water soluble monomers using 2D MoS2 as the mechanoredox catalyst, studied under various mechanical stimuli, including ultrasound, ball milling and low frequency vibrations. Our strategy enables complete polymerization within several minutes of work. This accelerated process can be utilized to create composite hydrogels with the ability to alter their mechanical and electrical properties in response to mechanical stimuli. This strategy has potential for applications in smart materials such as hydrogel sensors, artificial muscles, and implantable biomaterials. Mechanically controlled polymerization can lead to permanent changes in material structure, but material response can be slow. Here, the authors report the use of an MoS2 mechanoredox catalyst for the preparation of composite hydrogels with tuneable properties.