In the present work, tribological mechanisms under different sliding wear parameters, viz. applied load, sliding speed, and sliding distance, have been investigated in an Fe-based amorphous/ nanocrystalline coating synthesized by atmospheric plasma spraying. To understand the role of different wear parameters, Taguchi method was employed to design the experiments, and the results were analyzed using analysis of variance. The results revealed that sliding speed is the most significant contributing factor for wear rate of Fe-based amorphous/ nanocrystalline coating deposited by atmospheric plasma spraying process. A comprehensive understanding of influence of the sliding parameters on the wear process was understood based on different wear mechanisms. It was found that low sliding speeds resulted in predominantly abrasive wear, while high sliding speed led to mainly fatigue wear with a minor amount of abrasive wear. Interestingly, alterations in applied load and sliding distance did not induce a transformation in the wear mechanism itself; rather, they manifested in variations in the severity or extent of the wear mechanism. Increase in sliding speed and applied load led to an increase in the extent of wear loss, which was correlated with flash temperature on the coating surface and kinetic energy of the countermaterial during the wear process. On the contrary, increase in sliding distance caused a decrease in wear rate of the coating.