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We present combined in situ thermal cleaning and intentional doping strategies near the substrate regrowth interface to produce high-quality AlGaN/GaN high electron mobility transistors on semi-insulating (0001) GaN templates with low interfacial impurity concentrations and low buffer leakage. By exposing the GaN templates to an optimized thermal dissociation step in the plasma-assisted molecular beam epitaxy environment, oxygen, carbon, and, to lesser extent, Si impurities were effectively removed from the regrowth interface under preservation of good interface quality. Residual Si was further compensated by C-doped GaN via CBr4 to yield highly resistive GaN buffer layers. Improved N-rich growth conditions at high growth temperatures were then utilized for subsequent growth of the AlGaN/GaN device structure, yielding smooth surface morphologies and low residual oxygen concentration with large insensitivity to the (Al+Ga)N flux ratio. Room temperature electron mobilities of the two-dimensional electron gas at the AlGaN/GaN interface exceeded >1750 cm2/V s and the dc drain current reached ∼1.1 A/mm at a +1 V bias, demonstrating the effectiveness of the applied methods. [ABSTRACT FROM AUTHOR]