The emergence of zerovalent atom catalysts has been highly attractive for catalytic science. For many years, scientists have explored the stability of zerovalent atom catalysts and demonstrated their unique properties. Here, we describe an atom catalyst (AC) with atomically dispersed zerovalent molybdenum atoms on graphdiyne (Mo-0/GDY) with a high mass content of Mo atoms (up to 7.5 wt %) that was synthesized via a facile and scalable process. The catalyst shows both excellent selectivity and activity in the electrochemical reduction of nitrogen and in the hydrogen evolution reaction in aqueous solutions at room temperature and pressure. It is noted that this catalyst is the first bifunctional AC for highly efficient and selective ammonia and hydrogen generation. The catalytic process of our catalyst is well understood, the structure is defined, and the performance is excellent, providing a solid foundation for the generation and application of the new generation of catalysts.