Modern fuel-saving tire treads are commonly reinforced by silica due to the fact that this leads to lower rolling resistance and higher wet grip compared to carbon black-filled alternatives. The introduction of secondary fillers into the silica-reinforced tread compounds, often named hybrid fillers, may have the potential to improve tire performance further. In the present work, two secondary fillers organoclay nanofiller and N134 carbon black were added to silica-based natural rubber compounds at a proportion of silica/secondary filler of 45/10 phr. The compounds were prepared with variable mixing temperatures based on the mixing procedure commonly in use for silica-filled NR systems. The results of Mooney viscosity, Payne effect, cure behavior, and mechanical properties imply that the silica hydrophobation and coupling reaction of the silane coupling agent with silica and elastomer are significantly influenced by organoclay due to an effect of its modifier: an organic ammonium derivative. This has an effect on scorch safety and cure rate. The compounds where carbon black was added as a secondary filler do not show this behavior. They give inferior filler dispersion compared to the pure silica-filled compound, attributed to an inappropriate high mixing temperature and the high specific surface area of the carbon black used. The dynamic properties indicate that there is a potential to improve wet traction and rolling resistance of a tire tread when using organoclay as secondary filler, while the combination of carbon black in silica-filled NR does not change these properties.