NiTi shape memory alloy films were prepared by magnetron sputtering using a compound NiTi target and varying deposition parameters, such as power density, pressure, and deposition time. To promote crystallization, the films were heat treated at a temperature of 400 °C for 1 h. For the characterization, scanning electron microscopy, energy dispersive X-ray spectroscopy, atomic force microscopy, synchrotron X-ray diffraction, and nanoindentation techniques were used on both as-deposited and heat-treated films. Apart from the morphology and hardness of the as-deposited films that depend on the deposition pressure, the power applied to the target and the deposition pressure did not seem to significantly influence the characteristics of the NiTi films studied. After heat treatment, austenitic (B2) crystalline superelastic films with exceptionally high nickel content (~60 at.%) and vein-line cross-section morphology were produced. The crystallization of the films resulted in an increase in hardness, Young’s modulus, and elastic recovery.