Magnetoelectric (ME) coupling in Pb-based multiferroic composites has been widely investigated due to the excellent piezoelectric property of lead zirconate titanate (PZT). In this letter, we report a strategy to create a hybrid Pb-free ferroelectric and ferromagnetic material and detect its ME coupling at the nanoscale. Hybrid Pb- free multiferroic BaTiO3-CoFe2O4 (BTO-CFO) composite nanofibers (NFs) were generated by sol- gel electrospinning. The perovskite structure of BTO and the spinel structure of CFO nanograins were homogenously distributed in the composite NFs and verified by bright- field transmission electron microscopy observations along the perovskite [111] zone axis. Multiferroicity was confirmed by amplitude- voltage butterfly curves and magnetic hysteresis loops. ME coupling was observed in terms of a singularity on a dM/dT curve at the ferroelectric Curie temperature (T-C) of BaTiO3. The lateral ME coefficient was investigated by the evolution of the piezoresponse under an external magnetic field of 1000 Oe and was estimated to be alpha(31) = 0.78x10(4) mV cm(-1) Oe(-1). These findings could enable the creation of nanoscale Pb- free multiferroic composite devices. Copyright (C) EPLA, 2015