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Metallic glasses (MGs) have unusual structural characteristics and resulting unique properties, but effectively modulating their structure is difficult. The recently achieved two-way structural tuning (ordering-disordering) between distinct states in MGs offers an opportunity to overcome this challenge. However, pressures up to tens of GPa were required for the process, which limits sample sizes at the micrometer scale and challenges further comprehensive research. Here, by introducing concurrent shear straining with compressive force using high-pressure torsion, the pressure to trigger the disordering transition is significantly reduced to a few GPa. This enables the acquisition of millimeter-sized samples for comprehensive study, including synchrotron x-ray diffraction and small angle x-ray scatting, nanoindentation, electrical resistivity, and differential scanning calorimetry. It is evidenced that the two-way tuning of MG can be achieved both structurally and thermodynamically, which could help deepen our understanding of the mechanism behind the two-way tuning and promote exploration of distinct MGs. [Display omitted] [ABSTRACT FROM AUTHOR]