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We report a close correlation between the internal states and plasticity in a bulk metallic glass (BMG) and discover that the optimization of copper-mold casting current can induce large plasticity stably in an otherwise brittle BMG. It is possible to confirm that larger plasticity corresponds to the internal states with more average free volume (FV) as revealed by lower density, higher enthalpy change, and higher Poisson’s ratio. The enhanced plastic deformation mechanism is interpreted based on the FV model of BMGs, and our results may have some implications for understanding the role of the FV during plastic deformation of BMGs.