The ternary 0.52Bi2O3 – 0.18Fe2O3 – 0.30PbTiO3 (BFPT) system was prepared by mechanosynthesis in a high-energy planetary mill. The mixed powder was milled for 1, 2, 5, and 10 h. After 5 h of milling, the partially crystalline phase was achieved, as investigated by the XRD analysis. HRTEM verified the nanoparticle formation, and the mean size of the particles is estimated to be ⁓ 2.95 nm. Dielectric permittivity, loss tangent, electric modulus, and ac conductivity were measured for the milled system for 5 h as a function of frequency and temperature. The nanostructured BFPT sample shows a high dielectric permittivity (ε′ ⁓ 1388 at 500 Hz) obtained at Tc ⁓ 633 K (Curie temperature), which corresponds to the structural phase transition. The experimental results of σac are acceptable with the CBH model. The measurements of the P–E hysteresis loop illustrated recoverable energy density (Wrec=4.33 mJ/cm3) and energy storage efficiency (η=60.56%) at room temperature. The M-H data represent remnant magnetization (Mr) of 12.41 × 10−3 emu/g and coercive field (Hc) of 497.23 Oe. These remarks suggest that the nanostructured BFPT sample might be a promising option for magnetoelectric applications.