We design and synthesize nanostructured metal oxides and carbons using soft-chemistry methods. When prepared as aerogels and related pore-solid nanoarchitectures, these materials have the desirable properties of high surface area, continuous porosity, and a nanoscale solid network. The open pore structure of aerogels facilitates the transport of ions and molecules throughout the nanoarchitecture for interaction with the solid matrix. We also develop protocols to further modify such structures with biomolecules, polymers, metal colloids, ceramics, and semiconductors providing additional functionality and stability to the nanoarchitecture. These materials are targeted for a wide range of applications including batteries, fuel cells, catalysis, photovoltaics, sensors, and magnetics.