Pressure‐Tailored Energy State and Medium‐Range‐Order Structure in Fe‐Ni‐P Nanostructured Metallic Glass for High‐Sensitive Glucose Detection

Metallic glass has emerged as a promising electro‐catalytic material due to its metastable energy states and abundant undercoordinated sites. However, the limited capability to precisely manipulate its energy states and insufficient understanding of the energy‐structure‐property relationships hinder practical applications. Here, an innovative Laser‐IGC (laser ablation with inert gas condensation) synthesis strategy is developed by combining pressure‐controlled consolidation (1–5 GPa) to fabricate Fe‐Ni‐P nanostructured metallic glass with tunable atomic structure and energy states. Differential scanning calorimetry (DSC), X‐ray photoelectron spectroscopy (XPS), and surface wettability analyses reveal a consistent increase in energy state as consolidation pressure decreases. Pair distribution function (PDF) characterization discloses that pressure reduction induces atomic rearrangement at the medium‐range order (MRO) scale (3–5 Å), leading to optimized connectivity and packing density in the glassy matrix. The Fe‐Ni‐P nanostructured metallic glass consolidated at 1 GPa achieves outstanding glucose sensing performance with a high sensitivity of 1214.82 µA cm −2 m m −1 and ultra‐stability of 89% signal retention after 30‐day storage. This work preliminarily establishes a correlation between energy states and electro‐catalytic properties, while providing a novel pressure‐engineering pathway for designing high‐performance metallic glass catalysts.