A FeSiB nanoglass with improved alkaline hydrogen evolution performances is prepared by melt spinning followed by high-pressure torsion (HPT). HPT treatment induces slight unique crystallization meanwhile generates abundant interfaces/regions both inside the amorphous matrix and between the amorphous matrix and nanocrystallites. In 1.0 M KOH, the nanoglass requires an overpotential of only 112 mV to achieve the current density of 10 mA cm, which is much smaller than those of the corresponding amorphous alloy (385 mV) and crystalline alloy (465 mV). Furthermore, catalytic performance of the nanoglass remains almost unchanged after 50 h continuous reaction.