The influences of bentonite and different silane coupling agents (SCA) on the viscoelastic properties of nitrile butadiene rubber were studied in this work. The silane coupling agents compatibilized bentonite/nitrile butadiene rubber nanocomposites were fabricated by a novel green method. The viscoelastic behaviors of the nanocomposites and their vulcanizates were explored using a rubber processing analyzer (RPA) in the modes of strain sweep and frequency sweep. Storage modulus (G′) and elastic torque (S′) of nitrile butadiene rubber increased significantly with the incorporation of bentonite. In the SCA applied in this work, mercaptopropyltrimethoxysilane (MPTMS) contributed to high storage modulus (G′) of the nanocomposites because of thorough exfoliation of bentonite and short sulfur bonds formed during curing process. Meanwhile, multi-sulfur bonds in bis-[3-(triethoxysilyl)propyl] tetrasulfide (TESPT) and reversible interactions from [3-(2-aminoethylamino)propyl] trimethoxysilane (AEAPTMS) resulted in lower storage modulus of the cured nanocomposites.