Vladimir Tsukruk discusses recent results from his research group on designing robust, flexible, actuating, and responsive nanoscale multilayered hybrid nanomaterials for biosensing and bioelectronic applications. Ultrathin shells from synthetic and natural materials are assembled in order to conduct surface modification and protection of model microparticles, cells and cell assemblies. Microcapsules designed here are formed at interfaces from various linear and branched synthetic and biological macromolecules and graphene oxide assembled via hydrogen-bonding, ion pairing, and hydrophobic-hydrophobic interactions and tunable by temperature, pH or illumination of solutions. Various means are further exploited to transfer the LbL shells on various bacterial cells and place them in larger encapsulated cell arrays for bio-colometric detection. Ultra strong laminated bionanocomposites from silk and graphene oxide components with unique interphase morphology were found to possess extremely high elastic modulus and toughness, as well conductive patterning with localized electrochemical reduction.