A novel polymer electrolyte based on CsPbI quantum dots (QDs) reinforced polyacrylonitrile (PAN), named as PIL, is exploited to address the low room-temperature (RT) ion conductivity and poor interfacial compatibility of polymer solid-state electrolytes. After optimizing the content of CsPbI QDs, RT ion conductivity of PIL largely increased from 0.077 to 0.56 mS cm, and its Li-ion transference number ( ) from 0.20 to 0.63. It is revealed that the synergistic enhancement of Li-ion transport and interface stability is realized by CsPbI QDs through Lewis acid-base interaction, ordered polarization of PAN, and interface chemical regulation. These two effects guarantee the robust solid-electrolyte interface (SEI) in PIL-based solid-state batteries. Consequently, PIL electrolyte enables solid-state Li-metal batteries to deliver extraordinary RT cycling performance as verified by excellent cycling stability (>2000 h at 0.1 mA cm) of Li|PIL|Li symmetric batteries. Moreover, Li|PIL|LFP (LFP is LiFePO) and Li|PIL|NCM811 (NCM811 is Li(NiCoMn)O) batteries maintain capacity retention of 81.2% and 77.9%, respectively, after 600 cycles at 0.5 C, as well as good rate-capability and very high Coulombic efficiency at RT.
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