Silica is grown in situ into a natural rubber (NR)/chloroprene rubber (CR) blend (at 40/60 ratio), by a solution sol-gel method, where the silica content in rubber blend is increased in a controlled manner exceeding the limit found for the same blend ratio in the soaking sol-gel method. Reaction conditions have been optimized to get adequate conversion of tetraethoxysilane (TEOS, a silica precursor) to silica. Rheological, thermal, mechanical and viscoelastic properties of all the composites are compared with those of the unfilled rubber blend at similar conditions. Thermal and mechanical properties of the composites are found to improve consistently as silica content in the composite increases owing to increased rubber-filler interaction as revealed in dynamical mechanical analysis (DMA). Further improvement in the properties is observed for a particular composite where a silane coupling agent ((g-aminopropyl)trimethoxysilane, g-APS) is used in the reactive sol-gel system during in situ generation of silica. This is attributed to the uniform distribution of silica in the rubber matrix and strong rubber-filler interaction, caused by bifunctionality of silane, as revealed by morphology and DMA studies respectively. The reinforcement effect of silica is evaluated by comparing the experimental results with theoretical values obtained from the Guth-Gold model and the modified Guth model. The present study supplements the in situ silica generation in NR/CR blend of 40/60 ratio, following the solution sol-gel method, to the earlier study involving the soaking sol-gel method where the maximum reinforcement was found for this composition.