Morpho sulkowskyi butterfly wings contain naturally occurring hierarchical nanostructures that produce structural coloration. The high aspect ratio and surface area of these wings make them attractive nanostructured templates for applications in solar energy and photocatalysis. However, biomimetic approaches to replicate their complex structural features and integrate functional materials into their three-dimensional framework are highly limited in precision and scalability. Herein, a biotemplating approach is presented that precisely replicates Morpho nanostructures by depositing nanocrystalline ZnO coatings onto wings via low-temperature atomic layer deposition (ALD). This study demonstrates the ability to precisely tune the natural structural coloration while also integrating multifunctionality by imparting photocatalytic activity onto fully intact Morpho wings. Optical spectroscopy and finite-difference time-domain numerical modeling demonstrate that ALD ZnO coatings can rationally tune the structural coloration across the visible spectrum. These structurally colored photocatalysts exhibit an optimal coating thickness to maximize photocatalytic activity, which is attributed to trade-offs between light absorption and catalytic quantum yield with increasing coating thickness. These multifunctional photocatalysts present a new approach to integrating solar energy harvesting into visually attractive surfaces that can be integrated into building facades or other macroscopic structures to impart aesthetic appeal.