The discovery of novel materials that possess extraordinary optical properties are of special interest, as they inspire systems for next‐generation solar energy harvesting and conversion devices. Learning from nature has inspired the development of many photonic nanomaterials with fascinating structural colors. 2D photonic nanostructures, inspired by the attractive optical properties found on the inner surfaces of seashells, are fabricated in a facile and scalable way. The shells generate shining clusters for preying on phototactic creatures through interaction with incident solar light in water. By alternately depositing graphene and 2D ultrathin TiO2 nanosheets to form 2D–2D heterostructures and homostructures, seashell‐inspired nanomaterials with well‐controlled parameters are successfully achieved. They exhibit exceptional interlayer charge transfer properties and ultrafast in‐plane electron mobility and present fascinating nacre‐mimicking optical properties and significantly enhanced light‐response behavior when acting as photoelectrodes. A window into the fabrication of novel 2D photonic structures and devices is opened, paving the way for the design of high‐performance solar‐energy harvesting and conversion devices.