AbstractThe preparation of nanomaterials for energy applications such as intercalation batteries and materials that can act as substrates for water oxidation is a subject of major interest nowadays. In this work, we report the deposition of Prussian blue (PB) and its cobalt analogue (CoPBA) on mesoporous titania thin films (MTTF) using the successive ionic layer adsorption reaction (SILAR) technique under soft conditions. A bifunctional ligand, 1,10‐phenanthroline‐5,6‐dione (pd), was used to functionalize the titania surface and promote the growth of PB and CoPBA. The resulting PB@MTTF and CoPBA@MTTF nanocomposites were characterized using several techniques and it was determined that PB and CoPBA grow in a controlled and sequential manner, maintaining the mesoporous architecture. Both PB@MTTF and CoPBA@MTTF demonstrated very good electroactive properties, while CoPBA@MTTF exhibited water oxidation capabilities. The flexibility of this PBA@MTTF platform allows the incorporation of any labile transition metal ion or fragment into the structure of the coordination polymer embedded into a mesoporous matrix, opening the door for (photo)electrochemical devices and catalysts.