Magnetoelectric (ME) (CoFe2O4)(0.3)-(BaTiO3)(0.7) (CFO-BTO) nanostructures have been synthesized by a combinative using of hydrothermal reaction and polymer-assisted deposition. The feather-like nanostructures have an average diameter of 250 nm and lengths up to 5 mu m, with the single-crystal CFO nanopillars embedded in the BTO matrix. The CFO-BTO nanostructures exhibit good ferromagnetic and ferroelectric properties, as well as a large ME coefficient of 51.8 mV/cm Oe. A model has been proposed to explain the three-dimensional phases-connectivity of the nanostructures. And it is suggested that the novel type of phases-connectivity greatly promote the ME response. (C) 2010 Elsevier B.V. All rights reserved.