Integrating diamond with GaN high electron mobility transistors (HEMTs) improves thermal management, ultimately increasing the reliability and performance of high-power high-frequency 2 RF amplifiers. Conventionally, an amorphous interlayer is used before growing polycrystalline diamond onto the GaN in these devices. This layer contributes significantly to the effective thermal boundary resistance (TBReff) between the GaN HEMT and the diamond, reducing the benefit of the diamond heat spreader. Replacing the amorphous interlayer with a higher thermal conductivity crystalline material would reduce TBReff and help to enable the full potential of GaN-on-diamond devices. In this work, a crystalline Al0.32Ga0.68N interlayer has been integrated into a GaN/AlGaN HEMT device epitaxy. Two samples were studied, one with diamond grown directly on the AlGaN interlayer and another incorporating a thin crystalline SiC layer between the AlGaN and diamond.The TBReff, measured using transient thermoreflectance, was improved for the sample with SiC (30 ± 5 m 2 K GW -1 ) compared to the sample without (107 ± 44 m 2 K GW -1 ). The reduced TBReff is thought to arise from improved adhesion between the SiC and the diamond compared to the diamond directly on the AlGaN due to an increased propensity for carbide bond formation between SiC and diamond. The stronger carbide bonds aid transmission of phonons across the interface, improving heat transport.