Rechargeable aqueous Zn‐ion batteries (ZIBs) are always regarded as a promising energy storage device owing to their higher safety and durability. However, two problems have become the main trouble for the practical application of ZIBs such as the dendrite growth of Zn metal anode in electrolyte and the freezing of water solvent at low temperature. Herein, to overcome these challenges, a new strategy, multi‐component crosslinked hydrogel electrolyte, is proposed to inhibit Zn dendrites and realize low temperature environmental adaptability for ZIBs. Benefitting from the superior inhibition effect of the polyacrylamide and dimethyl sulfoxide (DMSO) on Zn dendrites, the coulombic efficiency of the symmetric cell of ≈99.5% is achieved during the Zn plating/stripping over 1 300 h, and the assembled full‐cell demonstrates the large specific capacity of 265.2 mAh g‐1 and high cyclic stability with the capacity retention of 95.27% after 3 000 cycles. In addition, the full‐cell delivers stable operation at a wide temperature range, from 60 to −40 °C, due to the introduction of additive DMSO. This work provides an inspired strategy and novel opportunities to realize a dendrite‐free and wide‐temperature rechargeable aqueous Zn‐ion energy storage system.

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excellent rate performance, and fast reaction kinetics. [1][2][3][4] However, the inadequate cycling performance of Zn metal anode (mainly including Zn foil) originates from the growth of Zn dendrites and other side reactions have impeded its further development and extensive commercialization. [5] To date, many efforts have been devoted to regulate the surface structure and characteristics of Zn foil to induce Zn nucleation and growth on the surface of Zn foil via various strategies such as surface coating of Zn foil and modification of electrolyte, [6][7][8] which have greatly enhanced the electrochemical performances of Zn foil. The inherent defects of planar Zn foil are always affecting its practical application, and there are three major factors involved: i) the 2D plane structure of Zn foil can cause spontaneous dendrite formation along the vertical direction on the surface of the Zn foil, which can easily penetrate the separator and cause short circuit of battery; ii) severe pulverization of Zn foil can occur during the charge/ discharge cycles at high current density, resulting in electric contact failure; and iii) the redundant thickness of Zn foil results in its poor utilization in application. [9,10] Compared with Zn foil, Zn powder (Zn-P) is a valuable substitute for Zn foil owing to its low cost and easily available. More importantly, the content of Zn-P can be accurately controlled, Zn powder (Zn-P)-based anodes are always regarded as ideal anode candidates for zinc ion batteries owing to their low cost and ease of processing. However, the intrinsic negative properties of Zn-P-based anodes such as easy corrosion and uncontrolled dendrite growth have limited their further applications. Herein, a novel 3D cold-trap environment printing (3DCEP) technology is proposed to achieve the MXene and Zn-P (3DCEP-MXene/Zn-P) anode with highly ordered arrangement. Benefitting from the unique inhibition mechanism of high lattice matching and physical confinement effects within the 3DCEP-MXene/Zn-P anode, it can effectively homogenize the Zn 2+ flux and alleviate the Zn deposition rate of the 3DCEP-MXene/Zn-P anode during Zn plating-stripping. Consequently, the 3DCEP-MXene/Zn-P anode exhibits a superior cycling lifespan of 1400 h with high coulombic efficiency of ≈9.2% in symmetric batteries. More encouragingly, paired with MXene and Co doped MnHCF cathode via 3D cold-trap environment printing (3 DCEP-MXene/Co-MnHCF), the 3DCEP-MXene/Zn-P//3DCEP-MXene/Co-MnHCF full battery delivers high cyclic durability with the capacity retention of 95.7% after 1600 cycles. This study brings an inspired universal pathway to rapidly fabricate a reversible Zn anode with highly ordered arrangement in a cold environment for micro-zinc storage systems.

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