The wide bandgap, high-breakdown electric field, and high carrier mobility makes GaN an ideal material for high-power and high-frequency electronics applications such as wireless communication and radar systems. However, the performance and reliability of GaN-based high electron mobility transistors (HEMTs) are limited by the high channel temperature induced by Joule-heating in the device channel. High thermal conductivity substrates (e.g., diamond) integrated with GaN can improve the extraction of heat from GaN-based HEMTs and lower the device operating temperature. However, heterogeneous integration of GaN with diamond substrates is not trivial and presents technical challenges to maximize the heat dissipation potential brought by the diamond substrate. In this work, two modified room-temperature surface-activated bonding (SAB) techniques are used to bond GaN and single crystal diamond with different interlayer thicknesses. Time-domain thermoreflectance (TDTR) is used to measure the thermal properties from room temperature to 480 K. A relatively large thermal boundary conductance (TBC) of the GaN-diamond interfaces with a ~4-nm interlayer (~90 MW/m 2 -K) was observed and material characterization was performed to link the structure of the interface to the TBC. Device modeling shows that the measured GaN-diamond TBC values obtained from bonding can enable high power GaN devices by taking the full advantage of the high thermal conductivity of single crystal diamond and achieve excellent cooling effect. Furthermore, the room-temperature bonding process in this work do not induce stress problem due to different coefficient of thermal expansion in other high temperature integration processes in previous studies. Our work sheds light on the potential for room-temperature heterogeneous integration of semiconductors with diamond for applications of electronics cooling especially for GaN-on-diamond devices.