Copper(I) thiocyanate (CuSCN) is a stable, wide bandgap (>3.5 eV), low-cost p-type semiconductor widely used in a variety of optoelectronic applications, including thin film transistors, organic light-emitting diodes, and photovoltaic cells. For CuSCN to have impact in the commercial fabrication of such devices, large-area, low-cost deposition techniques are required. Here, we report a novel technique for deposition of CuSCN that addresses these challenges. Aerosol-assisted chemical vapor deposition (AACVD) is used to deposit highly crystalline CuSCN films at low temperature. AACVD is a commercially viable technique due to its low cost and inherent scalability. In this study, the deposition temperature, CuSCN concentration and carrier gas flow rate were studied and optimized, resulting in homogeneous films grown over areas approaching 30 cm2. At the optimized values, i.e., 60 °C using a 35 mg/mL solution and a carrier gas flow rate of 0.5 dm3/min, the film growth rate is around 100 nm/min. We present a thorough analysis of the film growth parameters and the subsequent morphology, composition, and structural and optical properties of the deposited thin films.