In–Sn–Ga–O (ITGO) thin-film transistors (TFTs) fabricated by atomic layer deposition (ALD) are promising candidates for widespread semiconductor applications because of their high mobility and stability. To further improve the device characteristics, the doping efficiency of each cation must be increased. Here, we propose a facile method to enhance the device characteristics using plasma-enhanced ALD-nanocomposite (NC) structures. The deposition of SnO2 materials within the In2O3 layer of the ITGO film with the NC-ITO structure accelerates the reduction of In2O3 (In0: 35.3 % →46.1 %), thereby stabilizing SnO2 (Sn4+: 71.0 % →89.1 %). In addition, this process significantly decreases the fraction of oxygen-related defects (Odefect: 24.0 % →17.6 %) because Sn–O has a substantially higher bond dissociation energy than In–O. Consequently, the ITGO TFT with the NC-ITO active layer exhibits considerable improvements in the electrical parameters, such as an increase in the field-effect mobility from 41.9 to 54.5 cm2/V s and an enhancement in the subthreshold swing from 69.8 to 64.8 mV/decade. In addition, the device shows excellent results for negative bias illumination stress and positive bias temperature stress, with the differences in the threshold voltage shift being −0.22 and + 0.06 V, respectively.