Fe-doped LiTaO3 thin films with a low and high Fe concentration (labeled as LTO:Fe-LC and LTO:Fe-HC, respectively) were deposited by magnetron sputtering from two home-made targets. The dopant directly influenced the crystalline structure of the LiTaO3 thin films, causing the contraction of the unit cell, which was related to the incorporation of Fe3+ ions into the LiTaO3 structure, which occupied Li positions. This substitution was corroborated by Raman spectroscopy, where the bands associated with Li-O bonds broadened in the spectra of the samples. Magnetic hysteresis loops, zero-field cooling curves, and field cooling curves were obtained in a vibrating sample magnetometer. The LTO:Fe-HC sample demonstrates superparamagnetic behavior with a blocking temperature of 100 K, mainly associated with the appearance of Fe clusters in the thin film. On the other hand, a room temperature ferromagnetic behavior was found in the LTO:Fe-LC layer where saturation magnetization (3.80 kAm−1) and magnetic coercivities were not temperature-dependent. Moreover, the crystallinity and morphology of the samples were evaluated by X-ray diffraction and scanning electron microscopy, respectively.