We show that functionalizing polymer-coated colloidal nanoplatelets with guanosine groups allows synergistic increase of mechanical properties in nacre-mimetic lamellar self-assemblies. Anionic montmorillonite (MTM) was first coated using cationic poly(diallyldimethylammonium chloride) (PDADMAC) to prepare core-shell colloidal platelets, and subsequently the remaining chloride counterions allowed exchange to functional anionic 2'-deoxyguanosine 5'-monophosphate (dGMP) counterions, containing hydrogen bonding donors and acceptors. The compositions were studied using elemental analysis, scanning and transmission electron microscopy, wide-angle X-ray scattering, and tensile testing. The lamellar spacing between the clays increases from 1.85 to 2.14 nm upon addition of the dGMP. Adding dGMP increases the elastic modulus, tensile strength, and strain 33.0%, 40.9%, and 5.6%, respectively, to 13.5 GPa, 67 MPa, and 1.24%, at 50% relative humidity. This leads to an improved toughness seen as a ca. 50% increase of the work-to-failure. This is noteworthy, as previously it has been observed that connecting the core-shell nanoclay platelets covalently or ionically leads to increase of the stiffness but to reduced strain. We suggest that the dynamic supramolecular bonds allow slippage and sacrificial bonds between the self-assembling nanoplatelets, thus promoting toughness, still providing dynamic interactions between the platelets.