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Hydrogen energy has attracted sustainable attention in the exploitation and application of advanced power-generator devices, while the electrocatalysts for the hydrogen evolution reaction (HER) have been regarded as one of...

Along with the widespread utilization of hydrogen energy, the rise of highly active hydrogen evolution electrocatalysts with affordable costs presently becomes a substantial crux of this emerging domain. In this work, we demonstrate a feasible and convenient in situ seed-induced growth strategy for the construction of small-sized FeSe2 nanoparticles decorated on two-dimensional (2D) superthin Ti3C2T x MXene sheets (FeSe2/Ti3C2T x ) through a manipulated bottom-up synthetic procedure. By virtue of the distinctive 0D/2D heterostructures, abundant exposed surface area, well-distributed FeSe2 catalytic centers, strong surface electronic coupling, and high electrical conductivity, the resultant FeSe2/Ti3C2T x nanoarchitectures are endowed with a superior electrocatalytic hydrogen evolution capacity including a competitive onset potential of 89 mV, a favorable Tafel slope of 78 mV dec–1, and a long-period stability, significantly better than that of the pristine FeSe2 and Ti3C2T x catalysts.