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. Integration of GaN with high thermal conductivity substrates can improve the heat extraction from GaN-based HEMTs and lower the device operating temperature. However, heterogeneous integration of GaN with diamond substrates presents technical challenges to maximize the heat dissipation potential brought by the ultrahigh thermal conductivity of diamond substrates. In this work, two modified room-temperature surface-activated bonding (SAB) techniques are used to bond GaN and single crystal diamond. 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/m2-K) was observed and material characterization was performed to link the interfacial structure with the TBC. Device modeling shows that the measured TBC of the bonded GaN-diamond interfaces can enable high-power GaN devices by taking full advantage of the ultrahigh thermal conductivity of single crystal diamond. For the modeled devices, the power density of GaN-on-diamond can reach about 2.5 times as that of GaN-on-SiC and about 5.4 times as that of GaN-on-Si with a maximum device temperature of 250 oC. 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.