In the present work, the influences of different silane coupling agents (SCA) on the rheological behaviors of Bent/NBR nanocomposites during the curing process were investigated. The nanocomposites were prepared with a green method which is simple and free of organic solvents. The dispersion state and filler–polymer interfaces were analyzed with XRD, TEM, and SEM while rheological behaviors of the nanocomposites were explored with a rubber processing analyzer (RPA). (3‐Mercaptopropyl)trimethoxysilane (MPTMS) and bis[3‐(triethoxysilyl)propyl] tetrasulfide (TESPT) both improved the dispersion state of bentonite in the matrixes significantly. MPTMS increased the crosslinking density by forming single sulfur bonds while TESPT worked as a plasticizer and delayed the formation of crosslinking during curing process. [3‐(2‐Aminoethylamino)propyl]triethoxysilane (AEAPTMS) led to reversible filler–rubber interactions, which was the main reason for the low elastic torque of the vulcanized nanocomposites. J. VINYL ADDIT. TECHNOL., 25:236–242, 2019. © 2018 Society of Plastics Engineers