Recent efforts in nanoscience to control nanoparticles with atomic precision have met with success in solution-phase chemistry, opening new opportunities. The products, atomically precise nanoclusters (NCs), are not only compositionally well-defined but also structurally precise with unprecedented tailoring over the core and surface for specific functionalities. In this Perspective, we first highlight recent work in metal-hydride NCs for applications in catalytic hydrogenation and then reflect on the catalytic opportunities of atomically precise metal NCs. Metal NCs, as a new class of material, hold great promise for realizing the goals of understanding catalytic mechanisms at the atomic/molecular level (e.g., construction of active sites) and developing rules designing new catalysts with high activity and selectivity for important reactions. Tailoring NC catalysts at the atomic level will bring many exciting opportunities in future catalysis research.