To confirm the mechano-reactivity of camphanediol and demonstrate its application for selfstrengthening materials, we covalently incorporated these molecules into a promising polymer-double network (DN) hydrogels and investigated their capacity to generate more mechanoradicals and strengthen the materials. We modified cis-cyclohexanediol, pinanediol, and camphanediol into diacrylate crosslinkers and used them to synthesize poly(2-acrylamido-2-methyl-1-propanesulfonic acid) (PAMPS) single network (SN) hydrogels. These PAMPS networks with different crosslinkers serve as the first network in a DN hydrogel, with the second network identically consisting of polyacrylamide (PAAm) crosslinked with N,N'-methylenebis(acrylamide) (MBA) (Figure ). The resultant DN gels are denoted as DN-Cy, DN-Pin, and DN-Cam, respectively. Previous research has shown that DN systems are well-suited for studying mechanophore activation, where mechano-phore crosslinker with the lower activation force in the first network can be more efficiently and selectively activated. Figure and Figure show that the three SN gels and DN hydrogels exhibited similar swelling and mechanical properties, indicating comparable network structures. However, they displayed significant differences in generating reactive mechanoradicals. As shown in Figure and Figure , when the gels, fed with ferrous ions and xylene orange (XO), were stretched to a strain of 6 and then unloaded in air, DN-Cam exhibited a noticeable color change in the necked region, while DN-Cy and DN-Pin showed much weaker changes (see SI for a video clip). This color change occurs because the generated mechanoradicals oxidize ferrous ions to ferric ions in the presence of oxygen and water, and the ferric ions then react with xylenol orange to form a purple complex. Quantitative UV spectrum analysis revealed that DN-Cam generated approximately 130 µM mechanoradicals, over four times the amount produced by DN gels crosslinked with pinanediol and cis-cyclohexanediol, which generated around only 30 µM. We also investigated whether these mechanoradicals could trigger the polymerization of monomers and crosslinkers, endowing the gel with mechanoresponsive self-strengthening properties (Figure ). After oxygen extraction in a glove box for 2 hours, DN gels fed with 2.0 M monomer N-isopropylacrylamide (NIPAm) and 0.15 M crosslinker MBA were stretched to a strain of 6 and unloaded. After 3 minutes, DN-Cam turned white in its necked region and became stronger during a second cycle of loading-unloading test, while DN-Cy and DN-Pin did not. This suggests that a high concentration of mechanoradicals was generated in DN-Cam, facilitating the formation of a new PNIPAm network to strengthen the material.