Plasmonic metal/semiconductor heterostructures show promise for visible-light-driven photocatalysis. Gold nanorods (AuNRs) semi-coated with TiO2 are expected to be ideally structured systems for hydrogen evolution. Synthesizing such structures by wet-chemistry methods, however, has proved challenging. Here we report the bottom-up synthesis of AuNR/TiO2 nanodumbbells (NDs) with spatially separated Au/TiO2 regions, whose structures are governed by the NRs' diameter, and the higher curvature and lower density of CnTAB surfactant at the NRs' tips than on their lateral surfaces, as well as the morphology's dependence on concentration, and alkyl chain length of CnTAB. The NDs show plasmon-enhanced H2 evolution under visible and near-infrared light.