Multiferroic BiFeO3 (BFO) thin film exhibiting ferroelectric and enhanced magnetic properties was grown on La0.67Sr0.33MnO3 (LSMO) buffered Pt/TiO2/SiO2/Si substrates by off-axis RF magnetic sputtering, where a highly (111)-oriented texture was obtained. The BFO/LSMO thin film exhibits excellent ferroelectric and dielectric behavior (2Pr = 210.7 mu C/cm(2), 2Ec = 435 kV/cm, epsilon(r) = 116.8, and tan delta similar to 2.7% at 1 kHz), together with a long fatigue endurance up to 10(10) switching cycles at amplitude of 300 kV/cm. An enhancement in magnetic behavior was also observed with Ms = 89.5 emu/cm(3), which is largely contributed from the magnetic layer of LSMO. The coexistence of ferroelectric and ferromagnetic properties in the double layered BFO/LSMO thin film makes it a promising candidate system for applications where the magnetoelectric behavior is required. (C) 2011 The Electrochemical Society. [DOI: 10.1149/2.018202jes] All rights reserved.