TiO2 has garnered a flourish of interest in the field of energy storage and energy conversion. Herein, a new generation of 3D Ni foam supported in situ grown 1D TiO2 nanoarray (Ni/TiO2) is successfully prepared, through an easy solution‐phase hydrothermal process, and then CdS nanorods branched Ni/TiO2 nanoarrays are fabricated (Ni/TiO2@CdS). Their formation parameters and growth mechanism are carefully studied. Both Ni/TiO2 and Ni/TiO2@CdS monolithic catalysts exhibit advantaged photocatalytic (PC) and photoelectrocatalytic (PEC) water splitting properties compared with that of most previously reported TiO2‐based film photocatalysts. Mechanism investigation reveals that both type II and Z‐scheme charge transport mechanisms coexist in Ni/TiO2@CdS sample, and an additional Z‐scheme charge transfer effect accelerates the photogenerated charge separation and transport efficiency. This study may open a new avenue for the utilization of TiO2‐based film catalysts in a broader field of energy and environmental catalysis areas.
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