Highly donor-doped (110) layered perovskite materials loaded with nickel are efficient photocatalysts for overall water splitting with photon yields as high as 23% under UV irradiation. These novel photocatalysts are a series of homologous structures with a generic composition of A(m)B(m)O(3m+2) (m = 4, 5; A = Ca, Sr, La; B = Nh, Ti). The high electron density of these donor-rich materials would create a narrower charge depletion region of the semiconductor and an increased band bending, which allow more efficient electron-hole separation and higher quantum yields than undoped materials. Effects of catalyst preparation conditions are discussed on photocatalytic activity in water splitting.