We aimed to fabricate reliable memory devices using HfO2, which is gaining attention as a charge-trapping layer material for next-generation NAND flash memory. To this end, a new atomic layer deposition process using sequential remote plasma (RP) and direct plasma (DP) was designed to create charge-trapping memory devices. Subsequently, the operational characteristics of the devices were analyzed based on the thickness ratio of thin films deposited using the sequential RP and DP processes. As the thickness of the initially RP-deposited thin film increased, the memory window and retention also increased, while the interface defect density and leakage current decreased. When the thickness of the RP-deposited thin film was 7 nm, a maximum memory window of 10.1 V was achieved at an operating voltage of ±10 V, and the interface trap density (Dit) reached a minimum value of 1.0 × 1012 eV-1cm-2. Once the RP-deposited thin film reaches a certain thickness, the ion bombardment effect from DP on the substrate is expected to decrease, improving the Si/SiO2/HfO2 interface and thereby enhancing device endurance and reliability. This study confirmed that the proposed sequential RP and DP deposition processes could resolve issues related to unstable interface layers, improve device performance, and enhance process throughput.