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The unprecedented properties of multi-functional metastable β-Ti alloys, including superelasticity over a wide temperature range, ultra-low modulus, and Invar and Elinvar anomalies, have attracted a great deal of attention. Persistent research efforts have been made towards the understanding of the origins of these unique properties. In this article we report a novel shuffle-nanodomain regulated strain glass transition in a metastable β-Ti alloy, Ti-24Nb-4Zr-8Sn (wt.%, Ti2448), which could be the dominant transformation pathway that offers these unique properties. Using the ex-situ aberration-corrected scanning transmission electron microscopy and in-situ cooling transmission electron microscopy, we find that randomly distributed {011}< 0 1¯ 1> β O′ phase (orthorhombic, shuffle only) nanodomains embedded in the β phase (BCC) matrix at room temperature transform to α ″phase (orthorhombic) with a …