A dielectric composite with high dielectric constant, low dielectric loss and low percolation threshold was prepared by using the combined strategy of encapsulating of graphene oxide nanosheets (GONS) on carboxylated nitrile rubber (XNBR) latex particles and the in situ thermal reduction in GONS at a moderate temperature. The encapsulation of GONS on XNBR latex particles was mainly realized via the hydrogen bonding interactions between GONS and XNBR during latex mixing. A segregated graphene network was obtained at a low content of thermally reduced graphene (TRG), resulting in a low percolation threshold (0.25 vol.%). The dielectric constant at 100 Hz obviously increased from 23 for pure XNBR to 2211 and 5542 for the composite with 0.5 vol.% and 0.75 vol.% of TRG, respectively. The dielectric loss of the composites retained at a low value (less than 1.5). Meanwhile, the elastic modulus only slightly increased with the presence of 0.1-0.5 vol.% of TRG, keeping the good flexibility of the dielectric composites. This study provides a simple, low-cost and effective method to prepare high performance dielectric composites, facilitating the wide application of dielectric materials. (C) 2014 Elsevier Inc. All rights reserved.