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Glasses are typically characterized by time-dependent relaxation, leading to temporally changing properties. This inconsistency is a substantial issue in the development of new glasses, in particular optical glasses that require predictive responses to realize highly controlled and uniform optical responses. Here, we seek to expedite the relaxation rate using a novel thermo-ultrasonication process. As such, the As2S3 chalcogenide glass system is an ideal candidate due to its low glass-transition temperatures (Tg) and prevalent use as optical materials. The samples were subjected to ultrasonic vibration at an elevated temperature below Tg to accelerate their relaxation. We employ a combined theoretical–experimental approach to study glass relaxation via the evolution of refractive index and optical band edge. By understanding the effects of ultrasonication on glasses, we demonstrate new insights into the nature of relaxation while opening the possibility of developing ultra-stable glasses that can realize optical devices with increased lifespan.