The powder-mixed electric-discharge machining (PMEDM) process has been the focus of researchers for quite some time. This method overcomes the constraints of conventional machining, viz., low material removal rate (MRR) and high surface roughness (SR) in hard-cut materials, tool failure, and a high tool wear ratio (TWR). However, to determine the optimal machining parameter levels for improving MRR, surface finish must be measured during actual experimentation using various parameter levels across different materials. It is a very costly and time-consuming process for industries. However, in the age of Industry 4.0 and artificial intelligence machine learning (AI-ML), it provides an efficient solution to real manufacturing problems when big data is available. In this study, experimentation was conducted on AISI D2 steel using the PMEDM process for SR analysis with different parameters, viz. current, voltage, cycle time (TOn), powder concentration (PC), and duty factor (DF). Moreover, machine learning models were used to predict SR values for selected parameter levels in the PMEDM process. In this research, Gaussian process regression (GPR) with a squared exponential kernel, support vector machines, and ensemble regression models were used for computational analysis. The results of this work showed that Gaussian regression, support vector machine, and ensemble regression achieved 95%, 92%, and 83% accuracy, respectively. The GPR model achieved the best predictive performance among these three models.