The atomic composition ratio of solution-processed oxide semiconductors is crucial in controlling the electrical performance of thin-film transistors (TFTs) because the crystallinity and defects of the random network structure of oxide semiconductors change critically with respect to the atomic composition ratio. Herein, the relationship between the film properties of nitrate precursor-based indium-zinc-oxide (IZO) semiconductors and electrical performance of solution-processed IZO TFTs with respect to the In molar ratio was investigated. The thickness, morphological characteristics, crystallinity, and depth profile of the IZO semiconductor film were measured to analyze the correlation between the structural properties of IZO film and electrical performances of the IZO TFT. In addition, the stoichiometric and electrical properties of the IZO semiconductor films were analyzed using film density, atomic composition profile, and Hall effect measurements. Based on the structural and stoichiometric results for the IZO semiconductor, the doping effect of the IZO film with respect to the In molar ratio was theoretically explained. The atomic bonding structure by the In doping in solution-processed IZO semiconductor and resulting increase in free carriers are discussed through a simple bonding model and band gap formation energy.