High current pulsed electron beam (HCPEB) irradiation is an important surface engineering technique, which has been proved to be valid in modifying the surface microstructure and properties of various materials. In this work, HCPEB was employed to irradiate TiAlN coatings. The microstructure, mechanical and tribological properties of both original and irradiated TiAlN coatings were investigated. The results showed that the surface roughness of the TiAlN coatings first increased with 5 pulses of HCPEB irradiation, and then gradually declined with a further increase in pulse numbers. Compared with the original coating, the coating irradiated by 15 pulses demonstrated superior hardness (up to 33.4 GPa) and adhesion strength (112N), excellent wear resistance (wear rate of 3.3 × 10−6 mm3/Nm) and low friction coefficient (0.37). It is believed that the grain refinement, formation of the transition zone and adjustment of residual stresses after 15 pulses of HCPEB treatment are responsible for the improvement in both mechanical and tribological properties of the TiAlN coatings. These findings might suggest the potential applications of HCPEB irradiation for surface modification and hardness improvement of hard nitride coatings.