ZnO nanoparticles of 2.6 to 4.0 nm in size were interconnected by meso‐tetra(4‐carboxyphenyl)porphyrin (TCPP) for the realization of novel ZnO–TCPP networks, reaching lateral dimensions ranging from 50 to 800 nm. The resulting ZnO–TCPP networks were probed by dynamic light‐scattering experiments, transmission electron microscopy, and spectroscopy, and were also tested as photoactive top layers in TiO2 and ZnO dye‐sensitized solar cells (DSSCs). Control over these ZnO–TCPP networks on top of the semiconductor electrodes enables efficiency increases of 10 % and 46 % for TiO2‐ and ZnO‐based photoelectrodes, respectively. In other words, effects, such as reducing the electron recombination and increasing the electron lifetime, document the benefits of using tailored functional hybrid systems in DSSCs.