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The dye-sensitized photoelectrosynthesis cell (DSPEC) integrates high bandgap, nanoparticle oxide semiconductors with the light-absorbing and catalytic properties of designed chromophore–catalyst assemblies. The goals are photoelectrochemical water splitting into hydrogen and oxygen and reduction of CO2 by water to give oxygen and carbon-based fuels. Solar-driven water oxidation occurs at a photoanode and water or CO2 reduction at a cathode or photocathode initiated by molecular-level light absorption. Light absorption is followed by electron or hole injection, catalyst activation, and catalytic water oxidation or water/CO2 reduction. The DSPEC is of recent origin but significant progress has been made. It has the potential to play an important role in our energy future.