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Contact thermal resistance existed in the contact face between light emitting diode (LED) substrate and heat sink, which could hinder thermal conducting from PN junction to heat sinks, when mounting high power LEDs (HP-LEDs) devices on the heat sinks. Thermal interface materials (TIMs) were filled in the contact face to reduce contact thermal resistance. This paper studied the application of TIMs used in cooling LEDs, and three types of TIMs were studied by thermal test and optical-electro test. The experiment results presented that when select TIMs for LED mounting, thermal conductivity, thickness, and the volume of fillers should be considered.