Development of green tires by using silica and silane in tread compounds has emerged as a key technology in the tire industry. One of the most important features of a green tire is its low rolling resistance; however, agreement between other performances of a tire, such as wet grip and wear, along with rolling resistance of tread compounds, is a serious challenge. Properties of tire tread compounds are very sensitive to the silanization of silica and the loading of primary and secondary fillers. This work investigates simultaneous effects of silanization of silica as the primary filler and loading of carbon black as the secondary filler. By performing dynamic-mechanical testing in strain sweep and mechanical testing of tire tread compounds, the degree of silanization of silica and loading of carbon black were tuned to make agreement between friction, abrasion, and rolling resistance of green tire tread compounds. Morphology of the filler, kinetics of vulcanization, and bound rubber content in the tread compounds were used to explain the findings. Other than dynamic-mechanical analyses to predict final performance of tread compounds, direct measurements of friction, abrasion, and rolling resistance of tread compounds showed a 43% increase in the coefficient of friction on wet concrete, a 47% increase in abrasion resistance, and a rolling resistance coefficient of approximately 6.5 by using 10 parts per hundred of rubber (phr) of bis(triethoxysilylpropyl)tetrasulfide and 10 phr of carbon black N330 as the secondary filler.