The nickel-based complex Ni-CH3CH2NH2-intercalated niobate layered perovskite Ni-CH3CH2NH2/H1.78Sr0.78Bi0.22Nb2O7 was synthesized via a facile in situ chemical reaction method. Using ultrathin H1.78Sr0.78Bi0.22Nb2O7 nanosheets and nickel acetate as precursors. The composition, structure, photophysical properties, and photocatalytic activity for H-2 production of Ni-CH3CH2NH2/H1.78Sr0.78Bi0.22Nb2O7 were studied systematically. The photocatalyst loaded with 0.5 wt% Ni exhibited the highest H-2 evolution rate of 372.67 mu mo/h. This was 0.54 times higher than the activity of the H1.78Sr0.78Bi0.22Nb2O7 nanosheets. The activity of the optimized Ni-CH3CH2NH2/H1.78Sr0.78Bi0.22Nb2O7 was comparable to that of the Pt-loaded sample under the same reaction conditions. The photocatalytic activity of the Ni-CH3CH2NH2/H1.78Sr0.78Bi0.22Nb2O7 was mainly attributed to the excellent separation of photogenerated carriers, after formation of the intercalated complex Ni-CH3CH2NH2. This study provides a facile strategy to synthesize a non-precious metal-loaded photocatalyst for H-2 production.