The changes in the characteristics of plaster of Paris (pop) during drying operation under microwave irradiation conditions, namely surface morphology, effective moisture diffusivity, and absorption of microwave, were studied. The drying characteristics and kinetics of the process during microwave drying of plaster were studied for rectangular-faced cuboids (80 × 70 × 15, L × B × H in mm) through various drying parameters like microwave power input, initial moisture content, and drying time. Further, the experimental data on moisture ratio of plaster for different operating conditions were obtained and the optimization of the microwave drying process parameters was performed with response surface methodology (RSM) by considering all the above-said independent variables. Based on the RSM analysis, the optimum values of the process variables were obtained as: initial moisture content (A) 60%; microwave power input (B) 180 W; and drying time (C) 480 S.