Surface modified nanofillers are often used as curative-cum reinforcing agents for functional polymers. The polymer nanofiller interaction depends on the curative systems used. In the present study the carboxylic group of the carboxylated nitrile elastomer participated in the reaction with Zn-ion coated nanosilica filler producing a type of ionomeric elastomer. The interaction at the molecular level thus produced a high modulus vulcanizate. In this case, the S and MBT system, as curative, had an edge over the MDA and DPG curative system. Interfacial adhesion was enhanced in the presence of Zn-ion-coated nanosilica filler associated with dynamic mechanical behavior. The inferior properties obtained in the case of the MDA and DPG curative system were due to the decreased reactivity of the silica surface, thus reducing interfacial adhesion.