The addition of the active non-noble metal species on a ligand can influence the catalytic performance of catalyst. In the present work, a new bi-metallic solid-state complex catalyst system, including 4-4'-methylene bis(2,6-diethyl) aniline-3,5-di-tert-butylsalisilaldimin ligand and Fe and Co metal salts are prepared for hydrogen generation by catalytic hydrolysis of NaBH4. It was found that the Co/Fe mixture ratio, temperature, NaBH4, and NaOH concentrations, all exert considerable influence on the catalytic effectiveness of Co-Fe complex catalyst towards the hydrolysis reaction of NaBH4. The results suggested that the optimal mixture percentage of Co-Fe complex catalyst is 80:20. The obtained complex catalysts are characterized by XRD, FT-IR, and SEM techniques.