Fe-based amorphous coating is deposited on invar steel substrates using detonation spray and then through the cryogenic cycling (CCT) treatment from 0 to 60 cycles with the interval 10 cycles. Effects of CCT on microstructure, thermal properties, mechanical and tribological properties were investigated. It was found that, all the coated samples with CCT are still well bonded with the invar steel substrate, except for the surface of C60 appears local cracks. Moreover, it also found that although CCT did not significantly change the phase structure of the amorphous coating, CCT promoted the rejuvenation behavior in the amorphous coating, which also led to the heterogeneity of the internal structure. Attributed to this heterogeneity, it promotes the generation of a large amount of free volume in the amorphous coating, which results in a significant change in the toughness and resistance to crack propagation of the amorphous coating. And after 50 CCT cycles, the amorphous coating has undergone an obvious ductile-brittle transition, which has the highest fracture toughness K-IC and plastic work W-P value. The COF and wear rate of coatings increased initially, then followed by a decrease, but then again increased with the increase of CCT cycles. The 50-cycles coatings exhibited the lowest COF (0.60) and wear rate (0.56 x 10(-5) mm(3) N-1 m(-1)). The wear mechanism of all the samples is mainly delamination wear with oxidative wear, but the degree of delamination wear is obviously different, showing a trend corresponding to the tribological behavior of the amorphous coating. Therefore, the CCT method could be an effectively strategy to ameliorate the toughness and then enhance the wear performance of the Fe-based amorphous coating.