Hybrid electrocatalysts with excellent electrocatalytic activity for hydrogen reduction are fabricated using an efficient and facile electrochemical route. The electronic and synergistic effects between Co(OH)(2) and polyaniline (PANI) in the composite structure are the key factors that generate the high electrocatalytic activity and excellent stability. A highly efficient, non-precious metal-based flexible electrocatalyst for high-performance electrocatalysts is shown, which reveals a novel route for the design and synthesis of electrocatalysts.