The natural rubber (NR) nanocomposites were fabricated by filling ionic liquid (1-allyl-3-methyl-imidazolium chloride, AMI) modified nano-silica (nSiO 2 ) in NR matrix through mechanical mixing and followed by a cure process. Based on the measurements of differential scanning calorimetry (DSC), Fourier transform infrared spectroscopy (FTIR), solid state nuclear magnetic resonance spectroscopy, and Raman spectroscopy, it was proved that AMI could interact with nSiO 2 through hydrogen bonds. With the increase of AMI content, the curing rate of nSiO 2 /NR increased. The results of bound rubber and dynamic mechanical properties showed that polymer-filler interaction increased with the modification of nSiO 2 . Morphology studies revealed that modification of nSiO 2 resulted in a homogenous dispersion of nSiO 2 in NR matrix. AMI modified nSiO 2 could greatly enhance the tensile strength and tear strength of nSiO 2 /NR nanocomposites. Compared to unmodified nSiO 2 /NR nanocomposite, the tensile strength of AMI modified nSiO 2 /NR nanocomposite increased by 102%.