Novel, nanostructured electrode materials comprising porous ZnO films with aerogel morphology are presented. Almost any substrate including polymers, metals, or ceramics can be coated using a method that is suitable for mass production. The thin, porous films can be prepared from the wet gels via conventional drying, supercritical drying is not necessary. The filigree ZnO network is thermally very stable and exhibits sufficient electrical conductivity for advanced electronic applications. The latter was tested by realizing a highly desired architecture of organic-inorganic hybrid solar cells. After sensitizing of the ZnO with a purely organic squarine dye (SQ2), a nanostructured, interpenetrating 3D network of the inorganic semiconductor (ZnO) and organic semiconductor (P3HT) was prepared. The solar cell device was tested under illumination with AM 1.5G solar light (100 mW/cm(2)) and exhibited an energy conversion efficiency (η(eff)) of 0.69%.