This study investigates the nanoscale tribological characteristics of a Zr-based metallic glass (MG) after cryogenic cycling treatment (CCT). The MG, Zr63.6Cu18Ni10.4Al8, was subjected to different CCT cycles (0, 25, 50, 100, 200) to evaluate its tribological behavior. Atomic force microscopy (AFM) was used to perform nanoscale scratch tests, revealing that after 100 CCT cycles, the MG exhibited the highest adhesion and ploughing friction, but significantly improved anti-wear properties. Molecular dynamics simulations showed that the increased adhesion was due to the dominance of liquid-like regions in the CCT-treated MGs, while reduced hardness and weak elastic recovery led to deteriorated ploughing friction. Enhanced plasticity effectively dissipated strain from the AFM tip through multiple shear bands, weakening adhesion during deformation and improving wear resistance. The study highlights the beneficial effect of CCT on the anti-wear performance of MGs, providing insights for developing novel alloys. Previous studies have mainly focused on macroscopic tribological properties of MGs, with limited research on nanotribological performance affected by CCT. The emergence of AFM enables in-situ characterization of the heterogeneous structure and nanotribological properties of MGs. The results show that CCT enhances the anti-wear properties of MGs, offering new insights for tailoring wear-resistant MGs. The study also demonstrates the importance of CCT in exploring the nanotribological properties of MGs, especially in microdevice applications where conventional methods are no longer applicable. The findings suggest that CCT is a promising technique for improving the tribological performance of MGs.This study investigates the nanoscale tribological characteristics of a Zr-based metallic glass (MG) after cryogenic cycling treatment (CCT). The MG, Zr63.6Cu18Ni10.4Al8, was subjected to different CCT cycles (0, 25, 50, 100, 200) to evaluate its tribological behavior. Atomic force microscopy (AFM) was used to perform nanoscale scratch tests, revealing that after 100 CCT cycles, the MG exhibited the highest adhesion and ploughing friction, but significantly improved anti-wear properties. Molecular dynamics simulations showed that the increased adhesion was due to the dominance of liquid-like regions in the CCT-treated MGs, while reduced hardness and weak elastic recovery led to deteriorated ploughing friction. Enhanced plasticity effectively dissipated strain from the AFM tip through multiple shear bands, weakening adhesion during deformation and improving wear resistance. The study highlights the beneficial effect of CCT on the anti-wear performance of MGs, providing insights for developing novel alloys. Previous studies have mainly focused on macroscopic tribological properties of MGs, with limited research on nanotribological performance affected by CCT. The emergence of AFM enables in-situ characterization of the heterogeneous structure and nanotribological properties of MGs. The results show that CCT enhances the anti-wear properties of MGs, offering new insights for tailoring wear-resistant MGs. The study also demonstrates the importance of CCT in exploring the nanotribological properties of MGs, especially in microdevice applications where conventional methods are no longer applicable. The findings suggest that CCT is a promising technique for improving the tribological performance of MGs.