In this study, the properties of crystalline NdAlO3 thin films on n-type Si substrates at various pH values, preheating temperatures, and annealing temperatures were investigated. The grain size of NdAlO3 thin films increased with increasing annealing temperature and pH. In addition, it was also shown that porosity increased with a higher preheating temperature. At a preheating temperature of 300 °C, an annealing temperature of 800 °C, and pH 1.5, NdAlO3 films with a thickness of 65 nm were observed to have a dielectric constant of 24 at 1 MHz, a dissipation factor of 0.05 at 1 MHz, and a leakage current density of 3.9 × 10−7 A/cm2 at an electrical field of 30 kV/cm.