AbstractTitanium dioxide nanocomposites were synthesized in hierarchical architectures through the use of a 1,4‐dihydroxyanthraquinone photosensitizer. In the first step, the dye was either incorporated into the TiO2 core or adsorbed on its surface. In the subsequent phase, both structures were covered with an outer layer of titanium dioxide. The structure, morphology, aggregation, spectroscopic, and electrochemical properties of the synthesized TiO2‐based materials are presented with emphasis on the photosensitization and the photocurrent switching phenomena, which are also discussed within the context of the optical logic gates implementation and fuzzy logic systems operation. We present three different interpretations of the photocurrent action spectra yielding binary, ternary, or fuzzy logic circuits.