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Facile synthesis and application of nano-sized semiconductor metal oxides for optoelectronic devices have always affected fabrication challenges since it involves multi-step synthesis processes. In this regard, semiconductor oxides derived directly from metal–organic frameworks (MOFs) routes have gained a great deal of scientific interest owing to their high specific surface area, regular and tunable pore structures. Exploring the application potential of these MOF-derived semiconductor oxides systems for clean energy conversion and storage devices is currently a hot topic of research. In this study, titanium-based MIL-125(Ti) MOFs were used as a precursor to synthesize cobalt-doped TiO2-based dye-sensitized solar cells (DSSCs) for the first time. The thermal decomposition of the MOF precursor under an air atmosphere at 400 °C resulted in mesoporous anatase-type TiO2 nanoparticles (NPs) of uniform morphology, large surface area with narrow pore distribution. The Co2+ doping in TiO2 leads to enhanced light absorption in the visible region. When used as photoanode in DSSCs, a good power conversion efficiency (PCE) of 6.86% with good photocurrent density (Jsc) of 13.96 mA cm−2 was obtained with the lowest recombination resistance and the longest electron lifetime, which is better than the performance of the pristine TiO2-based photoanode. [ABSTRACT FROM AUTHOR]