Flexible scintillating fiber plays an important role in X‐ray radiation monitoring and high‐resolution medical imaging, while construction of scintillating fiber derived from the commercial material system meet with limited success. Here, we report the design and successful fabrication of the Ce‐activated lutetium aluminum silicate glass, nanostructured glass, and fiber, and explore their scintillating properties. The scintillating glass with optimized composition and optical properties is determined. The crystallization behavior of lutetium aluminum silicate glass is studied and the nanostructured glass embedded with orthorhombic Lu2Si2O7 phase is successfully constructed for the first time. Importantly, the crystalline layer thickness of the nanostructured glass can be finely tuned and ~172.89% enhancement in the scintillating performance can be achieved. Furthermore, the fiber with large sized core is fabricated and its radiation response properties are tested. The results show that it exhibits high sensitivity and its scintillating emission is lineally dependent on the X‐ray power, indicating the potential application for radiation detection.