In this paper, we study the sputter deposition and crystallization process to produce high quality Terfenol-D thin film (100 nm) with surface roughness below 1.5 nm. The Terfenol-D thin film was produced using DC magnetron sputtering technique with various sputtering parameters and two different crystallization methods, i.e. substrate heating and post-annealing. Several characterization techniques including WDS, XRD, TEM, AFM, SQUID and MOKE were used to determine the physical and magnetic properties of the Terfenol-D films. TEM studies reveal that the film deposited on the heated substrate has large grains grown along the film thickness producing undesirable surface roughness while the film crystallized by post-annealing method shows uniformly distributed small grains producing a smooth surface. The Terfenol-D film was also deposited onto (011) cut PMN-PT single crystal substrate. With the application of an electric field the film exhibited a 1553 Oe change in coercivity with an estimated saturation magnetostriction of λs = 910 x 10−6.