The development of high‐quality gallium nitride (GaN) epitaxy with thick drift layer, low controllable doping, and high mobility is key for vertical high‐power devices. Herein, the effect of increasing trimethylgallium (TMGa) molar flow rate on the growth rate, impurity incorporation, charge compensation, surface morphology, and carrier mobility is systematically studied. An optimized metalorganic chemical vapor deposition GaN growth condition with a typical growth rate of 2 μm h−1 is used as the baseline. With significant suppression of background Si, other impurity concentrations, and a precise control of the doping precursor SiH4 flow, an electron concentration as low as 4 × 1015 cm−3 in n−‐GaN is achieved. Through increasing the TMGa flow rate, the GaN growth rate is increased to 5.2 μm h−1. Secondary ion mass spectroscopy results show that the background H, O, and Mg remain below detection limit, but C level is increased to 2 × 1016 cm−3. GaN growth on Mn‐doped semi‐insulating GaN substrate is performed to probe the transport properties of film with low dislocation densities. Hall measurement shows that an electron mobility decreases from 852 to 604 cm2 V−1 s−1 as the growth rate increases. Results from this work reveal the challenge and guidance for achieving GaN vertical high power devices.