Plasma-enhanced atomic layer deposition (PEALD) is gaining interest in thin films for laser applications, and postannealing treatments are often used to improve thin film properties. However, research to improve thin film properties is often based on an expensive and time-consuming trial-and-error process. In this study, PEALD-HfO 2 thin film samples were deposited and treated under different annealing atmospheres and temperatures. The samples were characterized in terms of their refractive indices, layer thicknesses and O/Hf ratios. The collected data were split into training and validation sets and fed to multiple back-propagation neural networks with different hidden layers to determine the best way to construct the process-performance relationship. The results showed that the three-hidden-layer back-propagation neural network (THL-BPNN) achieved stable and accurate fitting. For the refractive index, layer thickness and O/Hf ratio, the THL-BPNN model achieved accuracy values of 0.99, 0.94 and 0.94, respectively, on the training set and 0.99, 0.91 and 0.90, respectively, on the validation set. The THL-BPNN model was further used to predict the laserinduced damage threshold of PEALD-HfO 2 thin films and the properties of the PEALD-SiO 2 thin films, both showing high accuracy. This study not only provides quantitative guidance for the improvement of thin film properties but also proposes a general model that can be applied to predict the properties of different types of laser thin films, saving experimental costs for process optimization.