This project brings together an interdisciplinary team of researchers with the aim to prepare novel and efficient functional materials to be used for metal-ion and pH sensing applications. Through a synergy in the synthetic, spectroscopic and computational techniques, we plan to focus our investigations on designing and characterizing a whole catalogue of compounds with desirable analytical and chemical features. Experimental work will involve traditional and ''click-chemistry'' strategies for the synthesis of a number of diverse benzimidazole, benzothiazole, 1,2,3-triazole, and coumarin derivatives, which will be incorporated into a range of organic, inorganic and hybrid polymeric matrices to form sensitive thin films or polymeric nanoparticles. Subsequently, through the UV/Vis and fluorescent spectroscopies, these will be assessed for their abilities to form both solution- and solid-phase complexes with metal cations in order to produce usable chemosensors. The choice of the metal analytes will be prompted by their biological significance or their presence in the environment, comprising cations such as Zn2+, Cu2+, Mn2+, Hg2+, Ag+, Cd2+, Fe2+/Fe3+, and Pb2+. All phases of experimental work will be supplemented with the computational support to aid in the interpretation of results. This will include calculating the conformational, tautomeric and pKa features of investigated systems, predicting the modes and free-energies of metal binding, and modeling the changes in the matching UV-Vis absorption and emission spectra induced by the metal complexation and solution pH variations. In addition, computations will be advanced by considering substituted derivatives of the prepared organic frameworks in order to fine-tune the preferred properties, thus helping in the guided selection of future directions. Overall, the presented research is intended to pose this team for the advancements in the field of chemosensors with the promise of a wide range of industrial applications.