An InAlN/AlGaN two-dimensional electron gas (2DEG) heterostructure with an "regrown AlN initial layer" was grown on AlN/sapphire template by metalorganic chemical vapor deposition, and their structural and electrical properties were investigated. It was confirmed that the prepared sample had an atomically-smooth heterointerface and exhibited an improved 2DEG mobility of 242 cm 2 /Vs compared to the sample without the regrown AlN layer.