An efficient chemical solution deposition (CSD) approach to growing epitaxial GaN layers at relatively low temperatures using a single-molecule precursor (SMP) is described. The precursor employed was bisazido diethylaminopropyl gallium, which exists as a dimer in the solid state and decomposes at relatively low temperatures. Using this precursor, epitaxial GaN layers were grown and characterized for their morphology, microstructure, and composition by X-ray diffraction (XRD), X-ray rocking curve (XRC) analysis, pole figure measurements, reciprocal space mappings, scanning electron microscopy (SEM), Rutherford backscattering (RBS), X-ray photoelectron spectroscopy (XPS), and room temperature photoluminescence (PL) measurements.