Provided are a method of depositing a thin film and a method of manufacturing a semiconductor device using the same, and the method of depositing a thin film uses a substrate processing apparatus including a chamber, a substrate support on which a substrate is mounted, a gas supply unit, and a power supply unit that supplies high-frequency and low-frequency power to the chamber, and includes: a step of mounting, on the substrate support, the substrate including a lower thin film deposited under the condition of a process temperature in a low temperature range; a step of depositing an upper thin film on the lower thin film under the condition of the process temperature in the low temperature range; and a step of treating a surface of the upper thin film under the condition of the process temperature in the low temperature range.