With an increased focus on light energy to facilitate catalytic processes, photocatalysts have been intensively studied for a wide range of energy and environmental applications. In this report, we describe the use of chemically dehydrated leaves as sacrificial foam-like templates for the growth of monolithic macrostructured semiconducting zinc oxide and nickel or cobalt doped zinc oxide materials. The composition and structure of these templated zinc oxides were characterized using X-ray powder diffraction, scanning electron microscopy, energy dispersive spectroscopy, and X-ray photoelectron spectroscopy. Optical properties were examined using solid-state UV–vis diffuse reflectance spectroscopy. The metal-doped ZnO materials have enhanced visible absorption and lower band gaps as compared to ZnO. The botanically templated ZnO materials retain the macroscopic cellular form of the leaf template with fused nanoparticle walls. Their UV photocatalytic oxidative abilities were investigated using methylene blue dye degradation in air. The leaf templated zinc oxides degrade ~85% of methylene blue dye with 30 min of UV illumination. Nickel and cobalt doped zinc oxides showed varying degrees of decreased UV and visible light photocatalytic activity, possibly due to metal-mediated charge recombination. The mild chemical dehydration process here allows complex soft botanical structures to be easily utilized for templating materials.