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The mechanical impact‐based energy harvesting characteristics of 0–3ϕBa0.85Ca0.15Zr0.10Ti0.90O3/(1−ϕ)polyvinylidene fluoride–polytetrafluoroethylene (BCZT/PVDF–PTFE); volume fraction (0 ≤ ϕ ≤ 0.25) nanocomposites, fabricated using a melt‐mixing method, are presented. A scanning electron microscope is utilized to investigate the distribution of BCZT nanoceramic powder as filler in the blended polymer (PVDF–PTFE; 80:20). The X‐ray diffraction method is applied to ascertain the formations of BCZT and BCZT/PVDF–PTFE. The values of apparent porosity, water absorption, shore D hardness, dielectric constant (εr), tangent loss (tan δ), piezoelectric charge coefficient (d33) and voltage constant (g33), and figure of merit (FM) are found to increase upon increasing ϕ. A significant increment in the impact‐generated electric voltage (25.38–77.73 V) and energy (9.42–243.9 nJ) is noticed with the increasing ϕ. In addition, the small values of water absorption (<0.091%) and tan δ (≈10−2) with relatively higher values of εr, d33, g33, FM, and shore D hardness, power out (Pdc = 0.47 mW using 470 Ω resistive load ϕ = 0.25 sample) as well as improved voltage generation and energy harvesting characteristics, prefigure the promise of the present composite system a superior lead‐free alternative for the applications in energy harvesting, detection/sensing, and structural health monitoring. [ABSTRACT FROM AUTHOR]