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Ni-rich Ni-Ti alloy thin films were fabricated by radio frequency (RF)-direct-current (DC) magnetron sputtering using elemental Ni and Ti as sputter targets. Si (100) was chosen as a substrate that was either held at room temperature or at 573 K (300 °C) during the depositions. The 380-nm-thick films were characterized by field emission scanning electron microscopy, energy dispersive spectroscopy, grazing incidence X-ray diffraction, atomic force microscopy, high-resolution transmission electron microscopy, and Vickers microhardness tester. The results suggests that because of the lack of surface mobility of the adatoms at the room temperature, the deposited films were smooth and amorphous, with a crystallite size of 15 nm accompanied with a porous morphology. At higher substrate temperatures, an increase in the surface diffusion leads to the formation of partially crystalline, rougher films with a denser, compact, fibrous grain microstructure. The formation of Ni-rich precipitates such as Ni4Ti3, Ni2Ti, and Ni3Ti along with small amount of the NiTi phase were attributed to the localized heating and cooling within the grains. Few grains exhibited band structures that are believed to be a result of type II twins.