Delafossite materials are considered to be a promising range of transparent conductive oxides for optoelectronic applications. The complications that have held back their implementation in practical devices lie in the complex growth methods that are required and in the formation of undesirable secondary phases. Herein, a fast, simple, and low-cost deposition method allowing the deposition of high-quality 2H-CuFeO 2 nanostructured thin films is employed. The effect of Sr doping on the properties of spray-coated CuFeO 2 thin film annealed at 850 °C is reported. X-ray diffraction (XRD) analysis revealed the delafossite structures of all the samples corresponding to the 2H-CuFeO 2 phase. The lattice spacing decreased with increasing substitution of Sr at the Cu site. Raman analysis further authenticated the structural results collected via XRD analysis. Surface scanning using field-emission scanning electron microscopy revealed the formation of nanostructured CuFeO 2 thin film possessing high crystalline quality, with the nanocrystal size increasing as the dopant content was increased. Energy-dispersive X-ray analysis allowed the quantification of the elements content via determining the ratios of the main elements as well as the dopant content in each sample. The optical properties of the samples showed strong light absorption in the visible region with a decrease in the band gap values with Sr insertion. First-principles calculations using density functional theory (DFT) were conducted to strengthen the experimental findings regarding the nature of the bonds in the hexagonal lattice of the CuFeO 2 compound and the effect of Sr doping on its characteristics. The electrical properties measured at room temperature revealed p-type conductivity with tunable resistivity, while the samples displayed increased electron mobility as a function of the dopant content. Consequently, our work introduced an efficient and cost-effective synthesis route for the preparation of high-quality nanostructured 2H-CuFeO 2 thin films, paving the way to facilitate further device applications., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)