Currently, it is still challenging to develop a hydrogel electrolyte matrix that can successfully achieve a harmonious combination of mechanical strength, ionic conductivity, and interfacial adaptability. Herein, we construct a multi‐networked hydrogel electrolyte with a high entanglement effect based on the gelatin/oxidized dextran/methacrylic anhydride, denoted as ODGelMA. Attribute to the Schiff base network formulation of −RC = N−, oxidized dextran integrated gelatin chains induce a dense hydrophilic conformation group. Furthermore, addition of methacrylic anhydride into this system through a grafting process, the entangled hydrogel achieves impressive mechanical features (6.8 MPa tensile strength) and high ionic conductivity (3.68 mS cm−1 at 20 °C). The ODGelMA electrolyte can not only regulate the zinc electrode by circumventing dendrite growth but also showcase an adaptable framework reservoir to accelerate the Zn2+ desolvation process on the Zn surface. Benefiting from the entanglement effect, the Zn anode achieves an outstanding average CE of 99.8% over 500 cycles and cycling stability of 900 h at 5 mA cm−2 and 2.5 mAh cm−2. The Zn||I2 full cell yields an ultra‐long cycling stability of 10000 cycles with a capacity retention of 92.4% at 5 C. Furthermore, a 60 mAh single‐layer pouch cell maintains a stable work of 350 cycles.This article is protected by copyright. All rights reserved