The introduction of end-chain functionalized rubbers, such as solution styrene-butadiene rubber (S-SBR), has enabled new approaches to enhance silica reinforcement in rubber. This study investigates hybrid core-shell silica-S-SBR particles, synthesized via ex situ coupling of end-chain functionalized S-SBR to silica, followed by hydrogenation. These hybrid particles were compared with non-hydrogenated S-SBR-modified silica in model tread compounds. Hybrid silica compounds showed reduced scorch time, less marching modulus and greater swelling due to the absence of double bonds, resulting in entanglement-based interactions rather than co-cross-linked interphase. These findings pave the way toward reversible, Velcro-inspired silica-rubber interactions, offering new design possibilities for dynamic applications.

• Modifications pathways of silica and functionalized rubber
• Co-crosslinking reinforcement
• Interactions via entanglements in hydrogenated S-SBR and silica