The material development of ternary alloy, AlGaN, is key to GaNbased device applications. This chapter includes a technical review of the key issues such as growth techniques suitable for AlGaN, microstructural analyses for extended defects and cracks accompanied with growth on foreign substrates, and the electrical and optical properties of AlGaN epitaxial films. Growth methods for the full range control of AI mole fraction in AlGaN have been introduced, together with a detailed discussion of bowing parameters in association with the determination of alloy band gap as a function of Al mole fraction.