In this study, artificial multiferroic Ba 0.85 Ca 0.15 Zr 0.1 Ti 0.9 O 3 /La 0.67 Ca 0.33 MnO 3 (BCZT/LCMO) epitaxial heterostructures were deposited on Nb-doped SrTiO 3 substrates using pulsed laser deposition. The epitaxial growth of the heterostructures on the substrate was demonstrated by XRD, RSM, and TEM analyses, which displayed decreasing residual strain with increasing BCZT layer thickness. The electrical, magnetic, and magnetoelectric properties of the epitaxial heterostructures were investigated in detail, and they were sensitive to the varying BCZT layer thickness in terms of residual strain. The multiferroic nature of the heterostructures was demonstrated by ferroelectric and ferromagnetic hysteresis loops. Strain-mediated magnetoelectric behavior was observed in the epitaxial heterostructures. Finally, dielectric properties were enhanced in the heterostructures over the BCZT single layer film, and the maximum magnetoelectric coefficient of the heterostructures was 206.5 mV/cm•Oe.