High-performance thin films combining large optical bandgap Al 2 O 3 and high refractive index HfO 2 are excellent components for constructing the next generation of laser systems with enhanced output power. However, the growth of low-defect plasma-enhanced-atomic-layer-deposited (PEALD) Al 2 O 3 for highpower laser applications and its combination with HfO 2 and SiO 2 materials commonly used in high-power laser thin films still face challenges, such as how to minimize defects, especially interface defects. In this work, substrate-layer interface defects in Al 2 O 3 single-layer thin films, layer-layer interface defects in Al 2 O 3 -based bilayer and trilayer thin films, and their effects on the laser-induced damage threshold (LIDT) were investigated via capacitance− voltage (C−V) measurements. The experimental results show that by optimizing the deposition parameters, specifically the deposition temperature, precursor exposure time, and plasma oxygen exposure time, Al 2 O 3 thin films with low defect density and high LIDT can be obtained. Two trilayer anti-reflection (AR) thin film structures, Al 2 O 3 /HfO 2 /SiO 2 and HfO 2 /Al 2 O 3 /SiO 2 , were then prepared and compared. The trilayer AR thin film with Al 2 O 3 / HfO 2 /SiO 2 structure exhibits a lower interface defect density, better interface bonding performance, and an increase in LIDT by approximately 2.8 times. We believe these results provide guidance for the control of interface defects and the design of thin film structures and will benefit many thin film optics for laser applications. KEYWORDS: plasma-enhanced atomic layer deposition, Al 2 O 3 single-layer thin film, Al 2 O 3 /HfO 2 /SiO 2 trilayer, laser-induced damage threshold, interface defect, interface bonding performance