Environmentally sustainable hydrogen‐evolving electrocatalysts are key in a renewable fuel economy, and ligand‐based proton and electron transfer could circumvent the need for precious metal ions in electrocatalytic H2 production. Herein, we show that electrocatalytic generation of H2 by a redox‐active ligand complex of Al3+ occurs at −1.16 V vs. SCE (500 mV overpotential). Two in one: Proton and electron transfer by a complex comprising Al3+ and a redox‐active iminopyridine ligand promotes electrocatalytic H2 evolution. The Al3+ center brings the reduction potential of the ligand into an accessible range for low‐overpotential proton production. The proposed mechanism involves two protonation events at the ligand and a subsequent two‐electron reduction to liberate hydrogen (see figure).