We have deposited bilayers of the FM La2/3Ca1/3MnO3 and FE BaTiO3 as a route to design systems with artificial magnetoelectric coupling. We have optimized the growth parameters for depositing LCMO/BTO/(001)Nb:STO by PLD at pure oxygen atmosphere and a substrate temperature of 820°C, keeping fixed the magnetic layer thickness (tLCMO~50 nm) and varying the thickness of the ferroelectric layer (tBTO=17.8, 44.4, 98.4 nm). Magnetization and transport measurements indicate possible multiferroic behaviour in the bilayer. We found an increase in the Curie and metal-insulator transition temperature in the bilayer in comparison with those for LCMO (48nm)/STO. Hysteresis loops on bilayers show ferromagnetic behaviour.