Multiferroic heterostructures composed of thin layers of ferromagnetic and ferroelectric perovskites have attracted considerable attention in recent years. We apply ab initio computational methods based on density functional theory to study the magnetoelectric coupling at the (0 0 1) interface between [Formula: see text] (LSMO) and [Formula: see text] (PZT). Our study demonstrates that the ferroelectric polarization of PZT has a strong influence on the distribution of magnetization in LSMO. The presence of polarized PZT changes the balance between the ferromagnetic and antiferromagnetic states of LSMO. The observed interfacial magnetoelectric effect can be explained by the variation of the charge density across the LSMO/PZT interface and by the change of the magnetic order in the LSMO layer adjacent to PZT.