Harnessing solar energy effectively by the judicious use of photoactive inorganic/hybrid structures has become a pivotal requirement in the pursuit of environmentally benign technologies. The synthesis of new inorganic materials whose stoichiometry, structure, and activity can be tuned while maintaining a high level of architectural homogeneity and the successful evaluation of each material as a viable component in specific energy-capture- and storage-based applications are being presented here. Two of our current projects are detailed, involving (i) new 1D-structured hybrid perovskite that is a more temporally and thermally stable analogue of the oft-cited methylammonium lead iodide and (ii) a new electroactive material that can function not only as a conventional electrode in a battery but also, because of the materials inherent photoactivity, as a component in solar batteries. Hence, the concept that energy capture and energy storage can be coupled in a single device is also being detailed.