Double-layered magnetoelectric thin films composed of Bi3.15Nd0.85Ti3O12 (BNT) and CoFe2O4 (CFO) were fabricated on Pt/Ti/SiO2/Si(1 0 0) substrates by chemical solution deposition with different growth sequences of BNT and CFO yielding the following layered structures: BNT/CFO/substrate (BC) and CFO/ BNT/substrate (CB). X-ray diffraction results reveal that there are no other impurity phases but BNT and CFO phases in both BC and CB thin films. Scanning electron microscopy observation shows BNT layer is more compact than CFO layer in the films. These double-layered films exhibit both good ferroelectric and magnetic properties, as well as magnetoelectric effects at room temperature. The layer sequences have a great effect on the magnetoelectric coupling behavior of these double-layered thin films, which may be caused by the interface bonding of BNT and CFO. (c) 2008 Elsevier B.V. All rights reserved.