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Abstract Some polymers are flexible, foldable, and wearable. Structural—functional composite is fabricated by adding inorganic fillers with functional properties. Up to date, compared with the polymer matrix, the composite prepared by polymer-inorganic fillers has lower flexibility, higher brittleness, and higher modulus of elasticity. In this paper, three-dimensional (3D) net-shaped submicron α-Al2O3, orthorhombic ZrO2, and rutile TiO2 fiber were fabricated by solution blowing spinning on a large scale. On the contrary, the elastic modulus (E) of the composite prepared by this 3D ceramic fiber was greatly reduced, and the flexibility of the composite was higher than that of the polymer matrix. When the strain was 75%, the E of the 3D net-shaped Al2O3 fiber-polydimethylsiloxane (PDMS) composite was 20% lower than that of PDMS. When the strain was 78%, the E of the 3D net-shaped TiO2 fiber-PDMS and 3D net-shaped ZrO2 fiber-PDMS composites decreased by 20% and 25%, respectively. This abnormal effect, namely the tunnel elastic enhancement effect, has great practical significance. In all-solid-state lithium-ion batteries, the composite inhibits lithium dendrite growth and the 3D inorganic network contributes to lithium ion transport. It is possible to promote the industrial production of low-cost and large-scale flexible solid-state lithium-ion batteries and it can enhance the energy storage density of energy storage materials. This novel idea also has bright prospects in flexible electronic materials.