Particulate matter (PM) emission is a serious drawback in several fields, threatening public health and the living environment worldwide. In the last decade, electrostatic interaction-based air filters have been developed owing to their effective filtration performance and low energy consumption. In this study, to develop ME-based electrostatic air filters, we developed polymer composites of poly(vinylidene fluoride-cotrifluoroethylene)/porous-Ni {P(VDF-TrFE)/p-Ni} by investigating the PM filtration efficiency and air flow resistance. P(VDF-TrFE)/p-Ni composites were prepared through a piezoelectric polymer coating of magnetostrictive p-Ni templates. In particular, to induce a sufficient surface charge in the composites for effective air filtering, the β-phase conformation and crystallization of P(VDF-TrFE) were enhanced by optimizing the dip-coating solutions. Moreover, the interfacial strain propagation between P(VDF-TrFE) and porous-Ni was investigated using varying weight ratios of P(VDF-TrFE)/p-Ni. Consequently, the ME-based composites with reusability were observed to exhibit maximum PM filtration efficiencies of 79.2% (PM 2.5 ) and 83.9% (PM 10 ) with a low pressure of 49 Pa. From the results, it was noted that the ME-based air filters of P(VDF-TrFE)/p-Ni can provide feasibility for more practical PM 2.5 removal of fine dust.