We report high surface area NanoCOT catalytic materials built on porous nickel foam for enhanced oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) of complete water splitting. Ni foam was coated with NanoCOT, a highly active material containing carbon, oxygen, and titanium. NanoCOT is synthesized and deposited on Ni foam from facile carbon thermal modification of Fe3+ treated P25 TiO2 nanoparticles in an atmosphere of methane, hydrogen, and nitrogen. Both the cathode and anode are prepared on Ni foam due to its high surface area and open 3D network structure. An alloy of NiMoZn was electrodeposited on Ni foam for HER. In addition to NanoCOT, electrodeposition of amorphous FeOOH was used to promote the oxygen evolution reaction (OER) on nickel foam in this study. The enhanced catalytic activities of the as-synthesized electrodes than previously reported NanoCOT electrode on planer substrate are attributed to the nanostructured COT electrode material and high surface area of Ni foam.