Rational design of noble catalysts with a potential to leverage efficiency at the atomic scale is vital for industrial applications. Such an ultimate atom-utilization efficiency can be achieved when all noble atoms exclusively contribute to catalysis. Here, we demonstrate a scalable synthesis of freestanding amorphous PtSex (where 1.2 < x < 1.3) layers acting as single-atom-layer of Pt catalysts with an unprecedentedly high atom-utilization efficiency (~ 30 wt%) at the monolayer limit. The amorphous PtSex behaviors a fully-activated surface accessible to catalytic reactions. The catalytic performance of the amorphous layer is featured by a nearly 100% current density relative to a pure Pt surface and reliable production of sustained high-flux hydrogen over a 2-inch sized wafer sample as a proof-of-concept. Furthermore, an electrolyser using the PtSex amorphous layer as a cathode is demonstrated to generate a high current density of 1000 mA cm− 2. Such an amorphization strategy is potentially extendable to other noble metals, including Pd, Ir, Os, Rh, and Ru elements, demonstrating the universality of single-atom-layer catalysts.