We show that the electrical and mechanical properties of the metal electrodes to the side walls of carbon nanotubes or graphene sheets can be dramatically improved through incorporation of (-CON-) and (-COO-) bifunctional molecular anchors. Thus for Pt, the (-CON-) anchor has a contact resistance 60 times lower than that of the simple nonanchored contact, while providing a much stronger mechanical linkage between the carbon and platinum metal contact. This should be useful for applications such as electronics, fuel cell catalysts, and spintronics.