The effect of a large amount of precipitated amorphous white silica nanofiller, pre-treated with bis[3-triethoxysilylpropyl-)tetrasulfide (TESPT), on the mechanical properties of a sulfur-cured natural rubber (NR) was studied. TESPT chemically adheres silica to rubber and also prevents silica from interfering with the reaction mechanism of sulfur-cure. The silica particles were fully dispersed in the rubber, which was cured primarily by using sulfur in TESPT, or, by adding a small amount of elemental sulfur to the cure system. The cure was also optimized by incorporating sulphenamide accelerator and zinc oxide into the rubber. The hardness, tear strength, tensile strength, and stored energy density at break of the vulcanizate were substantially improved when the filler was added. Interestingly, these properties were also enhanced when the rubber was cured primarily by using sulfur in TESPT.