This piece of contribution highlights the profound effect of unique mesoscale morphology of tailor made nanosilica assembly (SS-Silica), synthesized by sol–gel route, on the mechanical and dynamic rheological properties of platinum catalyzed addition-cured silicone elastomers. While commercial colloidal nanosilica (CS Silica) is used as the control nanofiller representing particulate morphology, the tailor-made SS-Silica having highly percolated network structure offers 10-fold increase in storage modulus of the uncured reactive PDMS precursor nanocomposite with stable dynamic rheological behavior and more than 180% enhancement in tensile strength of resulting liquid silicone rubber (LSR) produced on curing, as compared to colloidal silica of commercial origin. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014, 131, 40125.