The slow transition from an out-of-equilibrium glass towards a supercooled liquid is a complex relaxation phenomenon. In this Letter, we study the correlation between mechanical relaxation and equilibration kinetics in a ${\text{Pd}}_{20}{\text{Pt}}_{20}{\text{Cu}}_{20}{\text{Ni}}_{20}{\mathrm{P}}_{20}$ high-entropy metallic glass. The evolution of stress relaxation with aging time was obtained with an unprecedented detail, allowing us to pinpoint new interesting features. The long structural relaxation towards equilibrium contains a wide distribution of activation energies, instead of being just associated to the $\beta$ relaxation as commonly accepted. The stress relaxation time can be correlated with the equilibration rate and we observe a decrease of microstructural heterogeneity which contrasts with an increase of dynamic heterogeneity. These results significantly enhance our insight of the interplay between relaxation dynamics and thermodynamics in metallic glasses.

Fast development of metallic glass films with high toughness has been a long-sought goal of humankind in view of their superior properties and great potential for application in the field of soft electronics. However, until now, there has been no effective experimental strategy because of the lack of suitable and precise toughness measurement technology. In the present work, we introduced a feasible route for developing tough metallic glass films using combinatorial material library preparation and high-throughput toughness measurement via nanoindentation. Based on this route, tough metallic glass films for the quaternary Zr–Ti–Cu–Al system were successfully screened out. The corresponding electron work function map was detected to uncover the physical mechanism for the composition dependence of toughness. In addition, the preliminary assessments of the screened tough metallic glass films as strain-sensing materials were also conducted. Our current research not only provides a versatile toolbox for high-throughput development of tough metallic glass films, but also exemplifies their potential as strain-sensing materials.

Tuning structural heterogeneity in metallic glasses is key to improving their mechanical performance. Here we examine how carbon micro-alloying modulates the relaxation dynamics and creep of Fe-based amorphous ribbons. Increasing carbon content lowers the crystallization temperature, amplifies β-relaxation, and reduces hardness, consistent with enhanced atomic mobility. Nanoindentation creep, fitted with a stretched-exponential model, shows a decreasing exponent with carbon addition, indicating broader relaxation–time distributions and stronger dynamic heterogeneity. Nanoscale force-mapping further reveals a larger fraction of liquid-like regions and pronounced viscoelastic heterogeneity in carbon-rich samples. These changes facilitate the activation of shear-transformation zones and promote room-temperature creep flow. Together, the results establish a direct link between structural heterogeneity, relaxation processes, and mechanical response, providing guidance for the design of ductile metallic glasses.