•After the LSR, two surface modification zones (RZ and HAZ) with distinct microstructures appear in Zr-4 and N36.•Average hardness values of RZs of Zr-4 and N36 are ∼30% higher than their substrates.•Wear rates of the LSRed Zr-4 and N36 alloys are ∼30% and 18% lower than their substrates.•Compared with LSRed Zr-4, higher hardness and wear resistance of LSRed N36 is attributed to addition of 1 wt.% Nb. Two typical Zr alloys (Zr-4 and N36) for nuclear applications were surface-treated by laser surface remelting (LSR). Electron channeling contrast imaging and electron backscatter diffraction were used to characterize their main microstructure characteristics before and after the LSR, which were also correlated with their hardness and wear resistance. The results show that two surface modification zones with distinct microstructure characteristics appear in both the LSRed Zr alloys: (i) remelting zone (RZ) composed of fine α laths with dense internal nano-twins, and (ii) heat affected zone (HAZ) consisting of blocky α, lath α and second phase particles. The average hardness values of the RZs of Zr-4 and N36 alloys are 254.9 ± 8.5 HV and 269.5 ± 7.9 HV, respectively, ∼30% higher than their substrates. The wear rates of the LSRed Zr-4 and N36 alloys are found to be about 30% and 18% lower than their substrates, respectively, indicating significantly improved wear resistance. Comprehensive analyses reveal that refined grains, solid solution and internal nano-twins generated by ultrafast heating and cooling during the laser treatment have jointly led to the enhanced surface hardness of the LSRed Zr alloys, accounting for their improved wear resistance as well. Compared to the Zr-4 alloy, the refinement of the surface microstructure of the N36 alloy after the LSR treatment is more remarkable, contributing to higher hardness and wear resistance, which is mainly related to the addition of 1 wt.% Nb.