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The restacking tendency of 2D Ti 3 C 2 T X (MXene) sheets is the main obstacle preventing their application as functional materials in hydrogel. Herein, we fabricated novel ultra-stable 3D MXene-polyacrylamide (PAM) nanocomposite hydrogels inspired by the structure of a spider web. In particular, MXene nanosheets were uniformly located in a gel medium by precise alignment of sonication treatments, followed by the in-situ self-assembly of PAM hydrogel. In this instance, the MXene nanosheets are well-confined and trapped (via strong interactions) by the interwoven spider web-like structure of the PAM chains, which grow in-situ on the surface of the nanosheets. This approach proved effective to solve problems associated with the poor stability of MXene nanosheets in the hydrogel; more prominently, the tight cross-linked structure endows the MXene-PAM hydrogel with anti-compressive and anti-swelling capabilities; the continuous distribution of MXene nanosheets connected by the PAM network creates electron transport pathways and proton transport bridges in the hydrogel. Therefore, the hydrogel can be employed as a temperature and strain sensor or as a component of moist-electric nanogenerator. Image 1 • A temporary alignment and permanent in-situ fixation design was proposed. • Spider web-inspired anti-aggregation robust MXene hydrogel was constructed. • The DFT study predicts the formation for the bionic networks. • The hydrogel can be employed as sensor or moist-electric nanogenerator. [ABSTRACT FROM AUTHOR]