The present research aims to analyze the comminution behavior of ferrochrome slag using high-pressure grinding rolls. The laboratory bench scale high-pressure grinding rolls were used to study the three significant variables on the grinding efficiency of ferrochrome slag. The Central Composite Design was used to study the process variables, such as roll gap, applied load, and roller speed. The grinding efficiency was evaluated based on the product size and the energy consumption. The results showed that the increased gap between the rolls and roller speed decreases the product size with increased energy consumption. The results also found that an increase in applied load decreases the product fineness with increased energy consumption. The models were developed for the responses of P80 (size of 80% mass finer) and Ecs (specific energy consumption). Both the responses show high regression coefficients, thus ensuring adequate models with the experimental data. The minimum values of the P80 size and specific energy were determined using quadratic programming. The optimum values of the roll gap applied load and roll speed were found to be 1.43 mm, 16 kN, and 800 Rpm, respectively. The minimum values of P80 and the specific energy consumption were found to be 1264 µm and 0.56 kWh/t, respectively.