This study reports on the microstructure as well as dielectric and magnetoelectric properties of the Ba0.85Ca0.15Zr0.1Ti0.9O3/La0.67Ca0.33MnO3 (BCZT/LCMO) multiferroic heterostructure prepared by pulsed laser deposition. The XRD and TEM results identified the epitaxial growth of the heterostructure, and the interface between BCZT and LCMO was smooth without elemental inter-diffusion. The multiferroic nature of the BCZT/LCMO heterostructure was demonstrated by ferroelectric and ferromagnetic hysteresis loops. The enhanced multiferroic properties were achieved in the heterostructure as compared with single BCZT film, whose magnetoelectric coefficient was effectively promoted to 153.2 mV/cm.Oe.