A two-dimensional hole gas (2DHG) induced by polarization charges at the GaN/AlGaN hetero-interface is attracting much attention because of its potential to develop p-channel transistors required for GaN complementary logic integrated circuits. This platform is compatible with commercial AlGaN/GaN n-channel electronics, but the performance of GaN p-channel transistors has been far behind. In this work, 2DHGs in GaN/AlGaN/GaN heterostructures grown by plasma-assisted molecular beam epitaxy have been investigated. The Al composition of the AlGaN barrier has been pushed as high as possible without obvious strain relaxation, and the record high 2DHG sheet density and conductivity on the GaN/AlGaN/GaN platform have been obtained. By adopting a parallel conduction model, a dependent relationship of the 2DHG density on temperature has been extracted. The temperature dependent Hall-effect results have demonstrated that the 2DHG density boosts by 75 times and 46 times at room temperature and 77 K, respectively, when the Al composition is pushed from 0.18 to 0.45 for the AlGaN barriers. The 2DHG sheet density reaches 3.6 × 1013 and 2.1 × 1013 cm−2 at room temperature and 77 K, respectively, and the lowest sheet resistance is 8.9 kΩ/□ at 77 K. Such a 2DHG is beneficial for fabrication of p-channel GaN transistors with lower on-resistance on the already-industrialized platform.