The vulcanizate structure of silica-filled compounds is affected by the filler-rubber interaction (FRI) due to the silica-rubber coupling reaction and the chemical crosslink density (CCD) of the matrix rubber. In this study, the vulcanizate structure changes of silica-filled compounds according to the silane and sulfur variation were quantitatively analyzed using the Flory-Rehner and Kraus equations. In efficiency vulcanization (EV) conditions with low sulfur content, FRI increased when the bis-[3-(triethoxysilyl)propyl]tetrasulfide (TESPT) content increased, and the CCD clearly decreased. By contrast, in semi-EV conditions with high sulfur content, as TESPT content increased, the FRI increased the same way EV conditions, but the CCD was unchanged. Based on these results, it was confirmed that FRI of the silica-filled compounds increased as TESPT content increased, but CCD decreased or retained similar values according to the vulcanization system, indicating that the formation reaction of FRI was preferred over CCD.