SrTiO3 (STO) films are grown via atomic layer deposition at 370 °C with a two‐step growth method. A 5‐nm‐thick seed layer is first deposited and annealed via rapid thermal annealing (RTA) at temperatures ranging from 450 to 650 °C, and the main layer is subsequently grown on the annealed seed layer for in situ crystallization. When the RTA temperature is 500 °C or lower, the seed layer remains amorphous, and the main layer is also grown in the amorphous phase. At the 550 °C seed annealing temperature, the STO film is partially crystallized, and at the higher annealing temperature, the STO main layer is fully crystallized. The oxygen diffuses through the vertically aligned grain‐boundaries during the crystallized film growth, which induces the oxidation–reduction reaction of the underlying Ru substrate. This reaction causes a higher growth rate in the crystalline phase. The large growth rate difference between the amorphous and crystalline regions induces a severe roughening of the main layer. When RTA is done at 600 °C, the film is mostly crystallized, and the main layer becomes smooth again. Consequently, a 0.52 nm equivalent oxide thickness is achieved with the low leakage current of 2.5 × 10−8 A cm−2 at the 0.8 V applied bias.