Conversion and storage of solar energy into fuels and chemicals by artificial photosynthesis has been considered as one of the promising methods to address the global energy crisis. However, it is still far from the practical applications on a large scale. Nanoarray structures that combine the advantages of nanosize and array alignment have demonstrated great potential to improve solar energy conversion efficiency, stability, and selectivity. This article provides a comprehensive review on the utilization of nanoarray structures in artificial photosynthesis of renewable fuels and high value‐added chemicals. First, basic principles of solar energy conversion and superiorities of using nanoarray structures in this field are described. Recent research progress on nanoarray structures in both abiotic and abiotic–biotic hybrid systems is then outlined, highlighting contributions to light absorption, charge transport and transfer, and catalytic reactions (including kinetics and selectivity). Finally, conclusions and outlooks on future research directions of nanoarray structures for artificial photosynthesis are presented.