We present some facile routes to synthesize copper iodide (CuI) thin crystalline films and crystals. Using both hydrothermal and solvothermal techniques, particles at the nano/micro size are intrinsically produced on copper sheets by controlling the reaction between the sheet and iodine material under various parameters. The results are then characterized using scanning electron microscopy SEM, Xrays diffraction XRD and ellipsometry to obtain microstructural and optical properties, respectively. The thickness of the resulting film can be controlled by tuning working parameters such as temperature, concentrations of solvents, as well as time. The produced films/Crystals of CuI and can be used for different energy applications such as solar thermal collectors or photovoltaic cells, as the resulting microstructures possessed optical bandgaps ranging from 2.6-2.9 eV.