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Macroscopic self-assembly has increasingly attracted numerous concerns because of the facile fabrication of complex structures and diversified morphologies. Key challenges still remain to design high-performance building blocks to increase the efficiency and diversity of macroscopic self-assembly. Here, we designed triple noncovalent interactions (carboxyl-Zn 2+ coordination, host-guest interactions, and hydrogen bonding interactions) to enhance the interactions between self-healing fibers, constructing multidimensional nonwoven fiber-based fabrics through macroscopic self-assembly without further postprocessing. Profiled from the strong interactions generated from triple noncovalent interactions, ordered two-dimensional plane and three-dimensional spiral gel fabrics were fabricated using polyvinyl pyrrolidone/gel-based fibers as building blocks toward a human motion sensor. Moreover, we demonstrated that the macroscopic self-assembly strategy is universal to construct three-dimensional film-based fabrics toward wound dressing based on the triple noncovalent interactions between two-dimensional films. This macroscopic self-assembly approach provides an alternative strategy to fabricate gel fabrics for various applications.