Nanostructured materials-based research endeavors in renewable energy technologies play a dominant role in providing alternative solutions to the constraints of nonrenewable energy sources. Particularly, solar energy harvesting and solar water splitting are the two major hot cakes in the present state of the art in energy studies. In addition, the output of these studies can be the diversification of fuels with consistent power supplies. From the recent decades, the research in the field of solar photovoltaic technology has gained significant interest; while solar water splitting is in the emerging stage and hence many aspects from the materials used up to the scaling or modulation of the water-splitting devices have been obscure. Owing to their excellent optoelectrical properties, metal oxides have been established as a striking class among numerous semiconducting materials, and hence such materials can be extensively convenient for solar studies. However, the bare semiconducting metal oxides have various laggings concerning the further improvement in the efficiency of these energy technologies. To modify the bare metal oxides, metal–organic frameworks (MOFs) can show a vibrant role in composite formations, which is due to the superseding properties such as controllable architecture, adjustable pore size, high surface areas, and stability as well. Considering these aspects, this chapter is focused on nanostructured metal oxides/MOFs-based electrodes for solar energy harvesting and solar water splitting.