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Chemically sprayed indium-doped zinc oxide thin films (ZnO:In) were deposited on glass substrates starting from zinc pentanedionate and indium sulfate. The influence of both the dopant concentration in the starting solution and the substrate temperature on the transport, morphology, composition, linear and nonlinear optical (NLO) properties of the ZnO:In thin films were studied. The structure of all the ZnO:In thin films was polycrystalline, and variation in the preferential growth with the indium content in the solution was observed: from an initial (002) growth in films with low In content, switching to a predominance of (101) planes for intermediate dopant regime, and finally turning to a (100) growth for heavily doped films. The crystallite size was found to decrease with doping concentration and range from 36 to 23 nm. The film composition and the dopant concentration were determined by Rutherford backscattering spectrometry; these results showed that the films are almost stoichiometric ZnO. The optimum deposition conditions leading to conductive and transparent ZnO:In thin films were also found. In this way a resistivity of 4 × 10 −3 cm and an average transmittance in the visible spectra of 85%, with a (101) preferential growth, were obtained in optimized ZnO:In thin films.