The high thermal contact resistance (TCR) between the target and the heat exchanger in the Isotope Neutron Source Accelerator will cause the high-energy charged particle beam to stay in the target, resulting in a remarkable increase of temperature which affects the production of stable isotopes. At present, the usage of thermal interface materials (TIMs) can fill the gap at the contact surface and thus reduces the TCR. In this paper, aiming at the actual working condition of neutron source, the steady-state TCR measurement experiment is designed under vacuum and high temperature environment. The TCR at the contact surface was reduced after adding graphite films, thermal greases, liquid metals and preloads. The improvement of TCR of the contact surface between palladium (Pd), copper (Cu) and graphite (Gr) were measured respectively. The results show that the TCR between palladium and graphite is reduced by 95 % by adding liquid metal (Gallium alloy). The TCR between copper and graphite was reduced by 91 % by brazing method. Compared with other TIMs, graphite film has the advantages of high thermal conductivity, high temperature resistance and no fluidity. Adding 0.08 mm thick graphite film between Pd/Gr and Cu/Gr contact surface can reduce the TCR by 50 % and 70 %, respectively. The improvement effect between the two contact surfaces was not obvious when 15.9–318.3 kPa preload was applied.