Rejuvenation of metallic glasses, bringing them to higher-energy states, is of interest in improving their plasticity. However, how to achieve significant flow and rejuvenation throughout a deformed metallic glass remains challenging, and the mechanical behavior of the highly rejuvenated bulk metallic glasses is unexplored. In this presentation, we will reveal the significant improvement in compressive plasticity in a Zr-based bulk metallic glass (BMG) by structural rejuvenation, which is in stark contrast to the ageing induced brittleness. Upon constrained compression on the BMG rods at room temperature, extreme rejuvenation occurs in a large volume of BMG specimens, accompanied with a considerable amount of free volume generation, reduced hardness, Young’s modulus. As a result, shear transformation zones will be easily activated, giving rise to reduced yield strength of 1.37 GPa, much improved compressive plasticity, as well as more homogeneous deformation. The present work reveals the correlation between the deformation behavior and energy state in metallic glasses, which will help us to understand the deformation mechanism of metallic glasses, even disordered systems.