1 A g −1 under 0 °C with 95.24% capacity retention, which satisfies potential applications of wide‐ranging energy storage based on solid‐state ZIBs.22:T4cd,Abstract The zinc (Zn) anode in zinc‐ion batteries suffers from potential defects such as wild dendrite growth, severe Zn corrosion, and violent hydrogen evolution reaction, inducing erratic interfacial charge transfer kinetics, which eventually leads to electrochemical failure. Here, collagen, a biomacromolecule, is added to achieve the reconstruction of the electrolyte hydrogen‐bonding network and the modification of the derived Zn interface. Benefiting from the electronegativity advantage of amino groups (‐NH 2 ) in collagen, the Zn (002) crystal plane is preferentially exposed and the solid electrolyte interface (SEI) rich in ZnF 2 and Zn 3 N 2 promotes the rapid charge transfer of Zn anode. Thence, an impressive cumulative capacity of 7,500 mAh cm −2 at 30 mA cm −2 is achieved and the assembled Zn|VO 2 cell exhibited robust cycle reversibility even when subject to a maximum current of 100 A g −1 and an ultra‐long cycle life of 20,000 cycles at 50 A g −1 , with a single‐cycle capacity loss as low as 0.0021%. Such a convenient strategy of solvent sheathing regulation and derived interfacial manipulation opening up a promising universal approach toward long‐life and high‐rate Zn anodes.23:T46b,Parlous structure integrity of the cathode and erratic interfacial microdynamics under high potential take responsibility for the degradation of solid-state lithium metal batteries (LMBs). Here, high-voltage LMBs have been operated by modulating the polymer electrolyte intrinsic structure through an intermediate dielectric constant solvent and further inducing the gradient solid-state electrolyte interphase. Benefiting from the chemical adsorption between trimethyl phosphate (TMP) and the cathode, the gradient interphase rich in LiPF_xO_y and LiF is induced, thereby ensuring the structural integrity and interface compatibility of the commercial LiNi_0.8Co_0.1Mn_0.1O₂ (NCM811) cathode even at the 4.9 V cutoff voltage. Eventually, the specific capacity of NCM811|Li full cell based on TMP-modulated polymer electrolyte increased by 27.7% from 4.5 to 4.9 V. Such a universal screening method of electrolyte solvents and its derived electrode interfacial manipulation strategy opens fresh avenues for quasi-solid-state LMBs with high specific energy.

#	Concept	H-Index	Publications	Citations
1	Engineering	4	4	247
2	Chemistry	4	4	247
3	Materials Science	4	4	247
4	Chemical Engineering	2	2	110
5	Biomedical Engineering	1	1	31

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