As an empirical tool in materials science and engineering, the iconic phase diagram owes its robustness and practicality to the topological characteristics rooted in the celebrated Gibbs phase law (F = C – P + 2). When crossing the phase diagram boundary, the structure transition occurs abruptly, bringing about an instantaneous change in physical properties and limited controllability on the boundaries (F = 1). Here, we expand the sharp phase boundary to an amorphous transition region (F = 2) by partially disrupting the long‐range translational symmetry, leading to a sequential crystalline‐amorphous‐crystalline (CAC) transition in a pressurized In2Te5 single crystal. Through detailed in‐situ synchrotron diffraction, we elucidate that the phase transition stems from the rotation of immobile blocks [In2Te2]2+, linked by hinge‐like [Te3]2− trimers. Remarkably, within the amorphous region, the amorphous phase demonstrates a notable 25% increase of the superconducting transition temperature (Tc), while the carrier concentration remains relatively constant. Furthermore, we propose a theoretical framework revealing that the unconventional boost in amorphous superconductivity might be attributed to an intensified electron correlation, triggered by a disorder‐augmented multifractal behavior. These findings underscore the potential of disorder and prompt further exploration of unforeseen phenomena on the phase boundaries.This article is protected by copyright. All rights reserved