AbstractPolymer composite films are ideal materials for advanced energy storage capacitor in electrical systems. Therefore herein, we fabricated a novel series of polyvinylidene fluoride (PVDF) based composites embedded with well dispersed ZnO@APTES {surface modified zinc oxide with (3‐Aminopropyl) triethoxysilane (APTES)} nanoflake (0, 20, 30, 40, 50) vol% through solution casting method. Hydrothermally synthesized two‐dimensional ZnO was pre‐treated with H2O2 and surface modified with APTES for perfect distribution of nanoflake into PVDF matrix. Surface modification and high aspect ratio morphology of ZnO@APTES enhanced the interfacial interaction between organic PVDF and inorganic ZnO through reduction in heterogeneity between them. Surface functionalization reduced the dielectric loss and improved the overall energy storage performance. Investigation of electrical properties proclaimed incorporating 30 Vol% ZnO@APTES in PVDF as optimized loading due to its appreciable Wrec (recoverable energy density) about 3.2 J/cm3. Relative comparison of the energy storage density (Wrec) of PVDF/ZnO@APTES (30) vol% with recent published works established its enhanced capacitive response and its future application in energy storing portable device.