The most challenging requirement for depositing NiTi-based shape memory thin films is the control of film composition because a small deviation can strongly shift the transformation temperatures. This article presents a technique to control film composition via adjustment of the power supplied to the targets during simultaneous sputter deposition from separate Ni, Ti, and X (e.g., Hf) targets. After optimization of sputter parameters such as working gas pressure, target-substrate distance, and target power ratio, binary Ni100−xTix thin films were fabricated and characterized by energy dispersive x-ray spectroscopy in a scanning electron microscope (to measure the film composition and uniformity), in situ x-ray diffraction (to identify the phase structures), and differential scanning calorimetry (to indicate the transformation and crystallization temperatures). To explore the possibility of depositing ternary shape memory NiTi-based thin films with a high temperature transformation >100°C, a Hf target was added to the NiTi deposition system. Annealing was carried out in a high vacuum furnace slightly above the films’ crystallization temperatures (500 and 550 °C for NiTi and NiTiHf films, respectively). Differential scanning calorimetry (DSC) results of free-standing films illustrated the dependence of transformation temperatures on film composition: Ap and Mp (referring to the austenitic and martensitic peaks in the DSC curve) were above room temperature in near equiatomic NiTi and Ti-rich films, but below it in Ni-rich films. In NiTiHf films, the transformation temperatures were a function of Hf content, reaching as high as 414 °C (Ap) at a Hf content of 24.4 at. %. Atomic force microscopy revealed nanostructure surface morphology of both NiTi and NiTiHf films. Detailed characterization showed that the film properties were comparable with those of NiTi and NiTiHf bulk alloys.