The　basic　mantra　of　＂structure-dictates-function＂　in　chemistry　has　inspired　tremendous　interests　in　designing　various　architectures　toward　specific　applications.　In　this　work,　hierarchically　tailorable　double-array　structures　composed　of　TiO2　nanotube　arrays　(TNTAs)　and　axially　grown　ZnO　nanorod　arrays　(ZNRAs)　have　been　constructed　through　a　two-step　anodization　method　combined　with　a　heteroepitaxial　growth　process　regulated　by　electrodeposited　reduced　graphene　oxide　(RGO).　The　obtained　TNTAs/RGO/ZNRAs　film　hybrids　exhibit　enhanced　photocatalytic　and　photoelectrochemical　performances　along　with　favorable　photostability　as　compared　to　the　single　component　and　binary　counterparts.　This　is　ascribed　to　the　synergistic　effect　of　the　matchable　band　alignment　of　the　components,　the　1D-on-1D　double-array　architecture　with　vectorial　pathways　for　charge　carriers　transport,　and　the　electrically　conductive　RGO　for　bridging　the　directional　electron　flow　to　further　promote　the　separation　and　transfer　of　charge　carriers.　This　work　is　anticipated　to　provide　instructive　recipe　for　rational　design　and　construction　of　composite　films　with　optimized　photo(electro)catalytic　performances.