To further improve prediction accuracy and optimization quality of wire electrical discharge machining of SiCp/Al composite, trim cuts were performed using Taguchi experiment method to investigate the influence of cutting parameters, such as pulse duration (T on), pulse interval (T off), water pressure (W p), and wire tension (W t)), on material removal rate and three-dimensional surface characteristics (S q and S a). An optimization model to predict material removal rate and surface quality was developed using a novel hybrid Gaussian process regression and wolf pack algorithm approach based on experiment results. Compared with linear regression model and back propagation neural network, the availability of Gaussian process regression is confirmed by experimental data. Results show that the worst average predictive error of five independent tests for material removal rate, S q , and S a are not more than 10.66%, 19.85%, and 22.4%, respectively. The proposed method in this article is an effective method to optimize the process parameters for guiding the actual wire electrical discharge machining process.