Wear parameter optimization is critical for the successful use of materials in load-bearing applications. This study examines the optimization of various wear parameters using the Taguchi technique for the determination of the specific wear rate of alpha-manganese dioxide (α-MnO2)-epoxy nanocomposites. Four factors viz. wt.% loading of α-MnO2, sliding distance, sliding velocity, and normal load, were selected as controllable factors and a suitable L16 orthogonal array was chosen for conducting experiments. An X-ray diffractometer and field emission scanning electron microscope were used to examine phase identification, surface morphology, and chemical composition. With the addition of α-MnO2 in the epoxy, the tensile stress is decreased, while the elastic modulus is increased. The Taguchi result shows that the wear test in optimal condition is carried out with a wt.% loading of α-MnO2 of 0.5%, a sliding distance of 500 m, a sliding velocity of 1.5 m/s, and an applied normal load of 5 N. Analysis of variance shows the wt.% loading of α-MnO2 has the most influential parameter on specific wear rate with a contribution of 87.94%. The analysis also shows that the general linear model accurately describes the effect of sliding wear parameters on specific wear rates. The Monte Carlo simulated model shows that the experimental signal-to-noise ratios are consistent with the simulated model values. The confirmation test result shows that the % error between the predicted and experimental values of the specific wear rate at the optimum level combination is 4.67%. The worm surfaces of different trial runs show that the material removal process is caused by crack propagation. High-resolution scanning electron microscopic images of fractured surfaces show the formation of a stable tribo-layer at 0.5 wt.% α-MnO2 loading resulted in a significant decrease in the specific wear rate of the sample.