Multiferroic materials with robust magnetoelectric coupling at room temperature are of current research interest for their multifunctional device applications. Highly (100) oriented Pb(Fe0.5Ta0.5)x(Zr0.53Ti0.47)1-xO3 (PZTFTx) multiferroic thin films were deposited on La0.67Sr0.33MnO3 (LSMO) coated MgO (100) substrates using pulsed laser deposition technique. The film thicknesses were around 300 nm. X-ray diffraction analysis suggested tetragonal symmetry in these films at room temperature. Dielectric measurements on metal-ferroelectric-metal thin film capacitors were carried out between 100-106 Hz that revealed a broad dielectric peak maximum temperature at around Tm ~520 and 560 K for x = 0.2 and 0.3 films respectively, suggesting diffuse ferroelectric to paraelectric phase transition. The polarization-electric field (P-E) loop in the films exhibited a high saturation polarization of ~ 71 µC/cm2 and a large coercive field of 4.5 kV/cm, revealing its ferroelectric behavior. The thin films showed saturation magnetization of 8.3 (x =0.2), and 6.1 (x = 0.3) emu/cm3 at room temperature and had retained ferromagnetic/ferrimagnetic ordering at room temperature. The maximum magnetoelectric coupling in x =0.2 and 0.3 thin films were found to be 18.76 V/cm.Oe and 17.41 V/cm Oe respectively for in-plane bias field of around 350 Oe at room temperature, which are perhaps the largest values reported for single crystalline thin films and hence suitable for spintronic device applications.