Two-phase CoFe2O4 (CFO) and BaTiO3 (BTO) self-assembled nanocomposite thin films were fabricated by pulsed laser deposition. The epitaxial relationships between the CFO and BTO phases, and the substrate, were observed by transmission electron microscopy. Magnetoelectric (ME) coupling between the two phases was studied. We found a magneto-electro-chemical behavior, where induced charge can be used to deposit metal nanoparticles on the surface of films placed in an ionic solution. (C) 2011 The Electrochemical Society. [DOI: 10.1149/1.3573775] All rights reserved.