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Abstract: Developing novel materials for the conversion of solar to chemical energy is becoming an increasingly important endeavour. Perovskite compounds based on bandgap tunable oxynitrides represent an exciting class of novel photoactive materials. To date, literature mostly focuses on the characterization of oxynitride powder samples which have undeniable technological interest but do not allow the investigation of fundamental properties such as the role of the crystalline quality and/or the surface crystallographic orientation toward photo-catalytic activity. The challenge of growing high quality oxynitride thin films arises from the availability of a suitable substrate, owing to strict material and processing requirements: effective lattice matching, sufficiently high conductivities, stability under high temperatures and in strongly reducing environments. Here, we have established the foundations of a model system incorporating a TiN-buffer layer which enables fundamental investigations into crystallographic surface orientation and crystalline quality of the photocatalyst against photo(electro)chemical performance to be effectively performed. Furthermore, we find that TiN as current collector enables control over the nitrogen content of oxynitride thin films produced by a modified pulsed laser deposition method and allows the growth of highly ordered LaTiO3−xNx thin films.