The agglomeration of nickel‐coated graphite (NCG) in epoxy resin (EP) composites leads to low electrical conductivity of EP composites, which limits their development in electronic devices and multilayer circuits. In order to improve the electrical and thermal conductivity of NCG/EP composites, ethylenediamine (EDA) was used to modify NCG and compared with pure NCG‐filled EP composites. It was found that the conductive effect of modified composites with 20 wt% filler is better than that of unmodified composites with 40 wt% filler. The results of Fourier transform infrared spectroscopy and thermogravimetric analysis of EDA‐modified NCG (ENCG) showed that a coordination adsorption reaction occurred between EDA and NCG, forming N–Ni coordination bonds. When the filling amount of ENCG was 40 wt%, the conductivity and thermal conductivity of the composite are improved most significantly. The volume resistivity was reduced from 2.636 to 0.109 Ω cm, a decrease of 95.85%, and the thermal conductivity was improved from 0.517 to 0.968 W/(m K), an increase of 87.23%, respectively. Meanwhile, ENCG has better dispersion in the EP matrix than NCG.