The present paper discussed the development of a reliable and robust artificial neural network (ANN) capable of predicting the tribological performance of three highly alloyed tool steel grades. Experimental results were obtained by performing plane-contact sliding tests under non-lubrication conditions on a pin-on-disk tribometer. The specimens were tested both in untreated state with different hardening levels, and after surface treatment of nitrocarburizing. We concluded that wear maps via ANN modeling were a user-friendly approach for the presentation of wear-related information, since they easily permitted the determination of areas under steady-state wear that were appropriate for use. Furthermore, the achieved optimum ANN model seemed to be a simple and helpful design/educational tool, which could assist both in educational seminars, as well as in the interpretation of the surface treatment effects on the tribological performance of tool steels.