Efficient heat dissipation from electronic devices with high‐degree integration and high‐power density has become an urgent and complex problem. We report here novel thermal greases with an enhanced thermal conductivity using graphene flakes (GFs), hexagonal boron nitride (h‐BN), and hydroxypropyl cellulose (HPC) as fillers. The obtained GF/h‐BN/HPC thermal grease at 23 vol % h‐BN loading exhibits a thermal conductivity enhancement 555%, compared with the pure PDMS matrix, and also about 50, 169, and 115% higher than that with GF/h‐BN, h‐BN/HPC and h‐BN as the filler for the thermal grease, respectively. We attribute it to the synergistic effects among GF, h‐BN, and HPC, due to the formation of thermally conductive networks. This study provides a strategy for preparing thermal greases for thermal management applications. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019, 136, 47726.