Aluminium-doped zinc oxide (AZO) thin films were deposited via aerosol assisted chemical vapour deposition (AACVD) from zinc acetylacetonate and aluminium chloride at 450 °C. The precursor solutions consisted of methanol in a mixture with one other secondary solvent, including toluene, tetrahydrofuran, n-hexane, cyclohexane, and ethyl acetate. The crystal structures, elemental compositions and surface morphologies of the resulting AZO films were determined, as well as the optoelectronic properties. It was found that the more polar solvents enhanced growth in the (002) plane of the wurtzite crystal structure, and that solutions with low viscosities resulted in superior grain growth. The film deposited from a solution consisting of methanol and ethyl acetate displayed the lowest visible transmittance, due to carbon contamination. However, it also exhibited 60% lower resistivity, in comparison to the film deposited using methanol only. This suggests that optoelectronic properties can be tuned for specific photovoltaic devices.