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The emerging ultrawide-bandgap AlGaN alloy system holds promise for the development of advanced materials in the next generation of power semiconductor and UV optoelectronic devices. Within this context, heterostructures based on III-nitrides are very popular in view of their applications as electronic and optoelectronic components. AlGaN-based deep UV emitters are gaining visibility due to their disinfection capabilities. Likewise, high electron mobility transistors are attracting increasing attention owing to their superior electron transport which yields high-speed and high-power applications. These devices are conventionally made of AlGaN/GaN heterostructures grown on foreign substrates. However, structural defects, including stress induced by a mismatch in unit cell parameters and the presence of dislocations, can not only decrease the efficiency of the light emitters (by facilitating the non-radiative recombination of electron–hole pairs), but also impede electron mobility within the two-dimensional electron gas at the AlGaN/GaN interface. Therefore, the significance of obtaining high-quality AlGaN layers becomes evident. Including a thin AlN interlayer between the GaN buffer layer and AlGaN is a possible answer to address these drawbacks. Not only do we show that a thin AlN layer, approximately ≤3 nm in thickness, between the GaN buffer and AlGaN layers, is effective in decreasing the dislocation densities in the AlGaN layer by around 30%, but also this is responsible for an increase in the electron mobility (approximately 33%) compared to a classical AlGaN/GaN heterostructure. Additionally, the resulting heterostructure exhibits better optical quality, with a 7-fold increase in intensity as well as a 20% reduction in full-width at half-maximum in the AlGaN emission. [ABSTRACT FROM AUTHOR]