The U.S. Department of Energy recently announced its first Energy Earthshot on Clean Hydrogen, with a cost target of $1/kg-H₂ by 2031. Assuming future utility-scale grid electricity prices from photovoltaics ($0.02/kWh), 80% of the cost of H₂ would come from performing low-temperature water electrolysis at its thermoneutral voltage, with zero additional overpotential. This fact motivates alternative, less-expensive means of using light to generate mobile charge carriers than photovoltaics, and reactor designs with exceedingly low capital costs, like those we recently invented. Systems using low capital cost reactors benefit from low-voltage operation, which represents a paradigm shift from current state-of-the-art electrolyzers that aim to operate at high current densities. Analytical models predict that solar photocatalytic water splitting inherently operates at low voltages through use of an ensemble of optically thin photoabsorbers each operating at a low rate. Collectively the ensemble exhibits larger overall solar-to-hydrogen conversion efficiencies in comparison to optically thick designs. In efforts to attain these predicted higher efficiencies, we are performing detailed studies on the properties of state-of-the-art doped SrTiO₃ and BiVO₄ photocatalyst particles. During my talk, I will share our recent efforts in atomic-layer deposited ultrathin oxide coatings to impart redox selectivity and materials stability, single-photocatalyst-particle current–potential behavior and mobile charge carrier properties, and atomic-level information on dopant distributions and materials interfaces obtained from electron microscopies and X-ray spectroscopies. Collectively, our discoveries provide new design guidelines and additional research pathways for the development of effective composite materials to serve as active components in techno-economically viable artificial photosynthetic devices.