Flexible strain sensors have a wide range of applications in the field of health monitoring of seismic isolation bearings. However, the nonmonotonic response with shoulder peaks limits their application in practical engineering. Here we eliminate the shoulder peak phenomenon during the resistive-strain response by adjusting the dispersion of conductive nanofillers. In this paper, carbon black (CB)/methyl vinyl silicone rubber (VMQ) composites were modified by adding a silane coupling agent (KH550). The results show that the addition of KH550 eliminates the shoulder peak phenomenon in the resistive response signal of the composites. The reason for the disappearance of the shoulder peak phenomenon was explained, and at the same time, the mechanical properties of the composites were enhanced, the percolation threshold was reduced, and they had excellent strain-sensing properties. It also exhibited excellent stability and repeatability during 18,000 cycles of loading–unloading. The resistance-strain response mechanism was explained by the tunneling effect theoretical model analysis. It was shown that the sensor has a promising application in the health monitoring of seismic isolation bearings.