To achieve good interfacial interaction between fillers and rubber matrix is always a hot topic in rubber reinforcing industry. In this paper, acid activated bentonite (Bt) was alkalified to be alkaline calcium-bentonite (ACBt), then acrylic acid (AA) was employed to modify ACBt to obtain acrylic-bentonite (ABt). The results of Fourier transform infrared spectroscopy (FTIR) and X-ray diffraction (XRD) illustrated that acrylate groups were chemically boned onto the surface of Bt and the layer spacing of Bt was increased. During peroxide-induced vulcanization, in situ compatibilization of ABt was realized via the reaction between the unsaturated bonds of acrylate groups on the surface of Bt and the natural rubber (NR) chains. This resulted in an enhanced cross-linked network which contributed to the improved mechanical properties of NR/ABt composites. (C) 2015 Elsevier B.V. All rights reserved.