The temperature-dependent atomic structural evolution of a Zr64.13Cu15.75Ni10.12Al10 metallic glass is studied by in-situ high-energy X-ray diffraction in the temperature range of 79–553 K. The interatomic distance in the first nearest neighbor shell increases with decreasing temperature, while the interatomic distance in other atomic shells decreases. This decrease in the interatomic distances causes volume shrinkage and an increase in the strength of the metallic glass. The volume shrinkage can be quantitatively described by the Varshni function. The structural information is helpful for deeply understanding of the origin of the rejuvenation of metallic glasses at the cryogenic temperatures.