Functionalized carbon nanotubes (CNTs) were introduced into silicone grease to accompany the subsistent metallic oxide particles (micron-sized Al2O3, submicron-sized ZnO) with the aim of enhancing the thermal contact conductance of the composite grease as thermal interface materials (TIMs). The well-dispersed CNTs located among the metallic oxide particles to construct a three dimensional network structure and cooperated with them to form a highly efficient thermal transferring path. The functionalization of CNTs played a key role in achieving a good dispersion of CNTs in silicone grease matrix. The carboxylated CNTs were observed to show better dispersion in silicone grease and weaker reaction with oxide particles than pristine CNTs and amino-functionalized CNTs. Thus the thermal impedance of the silicone grease could be further decreased by 35% (as low as 0.18 cm(2) K/W) with the addition of 2 wt.% carboxylated CNTs. Finally, such CNT-modified silicone grease was used to enhance the performance of high-power light emitting diode and showed the prospective applications in TIMs. (C) 2013 Elsevier B.V. All rights reserved.