All inorganic perovskite quantum dots (QDs) have received great attention owing to their excellent performance in optoelectronic applications. However, they often suffer from defect-related photoluminescence (PL) quenching and phase transformation due to the loss of long-chain organic ligands, such as oleic acid (OA) and oleylamine (OAm). Here, we fabricated CsPbBr₃ QDs by a one-step microwave method, in the presence of α-phase poly(vinylidene fluoride) (PVDF) acing as the surface capping ligands. The PVDF-CsPbBr₃ QDs display a photoluminescence quantum yield (PLQY) of up to 98% (much higher than pristine QDs with OA/OAm as capping ligands), excellent stability in the desired cubic phase structure, and enhanced photoluminescence stability under ambient conditions. Using the as-prepared QDs as a light emitter, the efficient green perovskite quantum-dot light-emitting diode (QLED) with an external quantum efficiency (EQE) of 1.71% was prepared, exhibiting a peak luminance of 5711 cd m⁻² at 516 nm. Theoretical calculations indicate that there exists a much stronger interaction between the CsPbBr₃(001) surface and PVDF as compared to OA/OAm ligands, further explicating sufficient surface passivation with the introduced PVDF ligand.