There is considerable interest in broadband nanomaterials, particularly transparent semiconductor oxides, within both fundamental research and technological applications. Historically, it has been considered that the variation in dopant concentration during the synthesis of semiconductor materials is a crucial factor in activating and/or modulating the optical and structural properties, particularly the bandgap and the parameters of the unit cell, of semiconductor oxides. Recently, tin oxide has emerged as a key material due to its excellent structural properties, optical transparency, and various promising applications in optoelectronics. This study utilized the ultrasonic spray pyrolysis technique to synthesize aluminum-doped tin oxide (ATO) thin films on quartz and polished single-crystal silicon substrates. The impact of varying aluminum doping levels (0, 2, 5, and 10 at. %) on morphology and structural and optical properties was examined. The ATO thin films were characterized using scanning electron microscopy (SEM), X-ray diffraction (XRD), and transmittance spectroscopy. SEM images demonstrated a slight reduction in the size of ATO nanoparticles as the aluminum doping concentration increased. XRD analysis revealed a tetragonal crystalline structure with the space group P42/mnm, and a shift in the XRD peaks to higher angles was noted with increasing aluminum content, indicating a decrease in the crystalline lattice parameters of ATO. The transmittance of the ATO films varied between 75% and 85%. By employing the transmittance spectra and the established Tauc formula the optical bandgap values of ATO films were calculated, showing an increase in the bandgap with higher doping levels. These findings were thoroughly analyzed and discussed; additionally, an effort was made to clarify the contradictory analyses present in the literature and to identify a doping range that avoids the onset of a secondary phase.