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Modern data analytics techniques and computationally inexpensive software tools are fueling the commercial applications of data-driven decision making and process optimization strategies for complex industrial operations. In this paper, modern and reliable process modeling techniques, i.e., multiple linear regression (MLR), artificial neural network (ANN), and least square support vector machine (LSSVM), are employed and comprehensively compared as reliable and robust process models for the generator power of a 660 MW_e supercritical coal combustion power plant. Based on the external validation test conducted by the unseen operation data, LSSVM has outperformed the MLR and ANN models to predict the power plant’s generator power. Later, the LSSVM model is used for the failure mode recovery and a very successful operation control excellence tool. Moreover, by adjusting the thermo-electric operating parameters, the generator power on an average is increased by 1.74%, 1.80%, and 1.0 at 50% generation capacity, 75% generation capacity, and 100% generation capacity of the power plant, respectively. The process modeling based on process data and data-driven process optimization strategy building for improved process control is an actual realization of industry 4.0 in the industrial applications.