Developing cost-effective methods to synthesize large-size GaN films remains a challenge owing to the high dislocation density during heteroepitaxy. Herein, AlGaN/GaN HEMTs were grown on 6- and 8-inch Si(111) substrates using metal–organic chemical vapor deposition, and their basic properties and dislocation evolution characteristics were investigated thoroughly. With the insertion of a 100 nm thin AlGaN buffer layer, bow–warp analysis of the epitaxial wafers revealed excellent stress control for both the 6- and 8-inch wafers. HR-XRD and AFM analyses validated the high crystal quality and step-flow growth mode of GaN. Further, Hall measurements demonstrated the superior transport performance of AlGaN/GaN heterostructures. It is worth noting that dislocations tended to annihilate in the AlN nucleation layer, the thin AlGaN buffer layer, and the GaN buffer layer in the initial thickness range of 200–300 nm, which was indicated by ADF-STEM. To be specific, the heterointerfaces exhibited a significant effect on the annihilation of c-type (b = <0001>) dislocations, which led to the formation of dislocation loops. The thin inserted layers within the AlGaN buffer layer played a key role in promoting the annihilation of c-type dislocations, while they exerted less influence on a-type (b = 1/3<112¯0>) and (a+c)-type (b = 1/3<112¯3>) dislocations. Within an initial thickness of 200–300 nm in the GaN buffer layer, a-type and (a+c)-type dislocations underwent strong interactions, leading to considerable dislocation annihilation. In addition, the EELS results suggested that the V-shaped pits in the AlN nucleation layer were filled with the AlGaN thin layer with a low Al content.