Despite the excellent catalytic properties of individual nanoparticles and atomic clusters, the current capabilities to assemble them into a complex system are insufficient for many practical applications. An objective of this work is to develop a fabrication technology that allows for the simultaneous control of the nanoparticle surface chemistry, elemental distribution, microscale geometry, and large-scale assembly. Using a cellulose structure derived from wood, we fabricated hierarchical porous cellulose scaffolds combined with cerium-doped TiO2. This hybrid material served as the support for atomically dispersed Pt catalysts and was used to successfully decompose ethylene at zero degrees Celsius. The fabrication concept developed in this work would allow mitigating the conflict between the required large active surfaces and the difficulties in handling nanopowders in environmental catalysis, including food preservation and indoor air purification. We thus discovered a promising route to manufacture multifunctional materials with complex structures by combining a controllable chemical synthesis with the nature-designed wood scaffold.