Display omitted •Sonication assisted destartification to pristine grapheme has been synthesised.•In situ nanocomposite hydrogel is mechanically robust, highly stretchable, rubber-like elastic and reversibly ductile.•Prepared hydrogel showed conductivity and promoted as dual responsive (pH and electric impulse) controlled release device.•Hydrogel is non-toxic and shows superior result in live-dead assay. Nanohybrid hydrogels based on pristine graphene with enhanced toughness and dual responsive drug delivery feature is opening a new era for smart materials. Here pristine graphene hydrogels are synthesized by in situ free radical polymerization where graphene platelets are the nanobuiliding blocks to withstand external stress and shows reversible ductility. Such uniqueness is a mere reflection of rubber-like elasticity on the hydrogels. These nanobuilding blocks serve also the extensive physisorption which enhances the physical crosslinking inside the gel matrix. Besides the pH-responsive drug release features, these hydrogels are also implemented as a pulsatile drug delivery device. The electric responsive drug release behaviours are noticed and hypothesized by the formation of conducting network in the polyelectrolytic hydrogel matrix. The hydrogels are also tested as good biocompatibility and feasible cell-attachment during live-dead cell adhesion study. The drug release characteristics can also be tuned by adjusting the conducting filler loading into the gel matrix. As of our knowledge, this type of hydrogels with rubber-like consistency, high mechanical property, tunable and dual responsive drug delivery feature and very good human cell compatible is the first to report.