4,4‐diphenylmethane diisocyanate‐modified graphene oxide (GO) was fabricated (GO‐NCO), and for the first time used to reinforce the nitrile‐butadiene rubber (NBR) by using latex compounding approach. The modification process was verified by employing the Fourier transform infrared spectroscopy, X‐ray photoelectron spectroscopy, X‐ray diffraction, and field‐emission transmission electron microscopy. The morphologies of the fracture surfaces of the NBR and its nanocomposites were analyzed using high‐resolution scanning electron microscopy. The mechanical properties, dynamic rheological properties and the thermo‐physical properties of the NBR/GO‐NCO nanocomposites were compared and investigated. At same filler concentration, the NBR/GO‐NCO nanocomposites exhibited the superior performances than the NBR/GO nanocomposites did. The NBR/GO‐NCO exhibited the highest tensile strength of 8.3 MPa, which was almost 200% higher than that of the neat NBR composites. And the storage modulus continuously enhanced with the filler concentration attributing to the enhanced stiffness due to the GO‐NCO in the rubber matrix. POLYM. COMPOS., 40:E1103–E1110, 2019. © 2018 Society of Plastics Engineers