Multilayer composite solid electrolytes (CSEs) exhibit many advantages over uniform monolayer CSEs but are hindered by high interlayer resistance and complex preparation methods. Herein, for the first time, a natural sedimentation strategy was developed to construct concentration gradient CSEs (GCSEs) for lithium-metal batteries (LMBs). This method utilizes intrinsic gravity and photopolymerization to achieve multiple functions in the monolayer, avoiding additional interlayer resistance and reducing preparation time. Owning to the concentration gradient structure, the Li+ transport on the PolyIL-rich side relies on the weak solvation of Li+ with EMIMTFSI, while the Li+ transport on the LLZTO-rich side follows the 'vehicular diffusion' mechanism with the aid of TFSI−, improving the Li+ transport and enhances the Li+ transference number, leading to the high stability to 2300 h for the Li//Li cell and stable operation at 4.3 V with 89.6 % capacity retention after 100 cycles for the assembled LMB. Moreover, compared with the monolayer uniform hybrid CSEs, the gradient structure alleviates uncoordinated thermal expansion between LLZTO and PolyIL, avoiding stress increase during cycling and battery capacity fade. This gradient strategy mitigates high interlayer resistance and offers a universal path to address the sluggish Li+ transportation in multilayer CSEs and improves compatibility between the electrolyte and electrodes in fabricating solid-state batteries.

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