Single‐atom catalysts (SACs) have been one of the frontiers in the field of catalysis in recent years owing to their high atomic utilization and unique electronic structure. To facilitate the practical application of single‐atom, it is vital to develop a sustainable, facile single‐atom preparation method with mass production potential. Herein, a universal one‐step electrochemical synthesis strategy is proposed, and various metal–organic framework‐supported SACs (including Pt, Au, Ir, Pd, Ru, Mo, Rh, and W) are straightforwardly obtained by simply replacing the guest metal precursors. As a proof‐of‐concept, the electrosynthetic Pt‐based catalysts exhibit outstanding activity and stability in the electrocatalytic hydrogen evolution reaction (HER). This study not only enriches the single‐atom synthesis methodology, but also extends the scenario of electrochemical synthesis, opening up new avenues for the design of advanced electro‐synthesized catalysts.