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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.