Most synthetic processes of metallic nanostructures were assisted by organic/inorganic or polymeric materials to control their shapes to one-dimension or two-dimension. However, these additives have to be removed after synthesis of metal nanostructures for applications. Here we report a straightforward method for the low-temperature and additive-free synthesis of nanobelt-like silver nanostructures templated by nanocarbon (NC) materials via bio-inspired shape control by introducing supramolecular 2-ureido-4[1H]pyrimidinone (UPy) groups into the NC surface. The growth of the Ag nanobelt structure was found to be induced by these UPy groups through observation of the selective formation of Ag nanobelts on UPy-modified carbon nanotubes and graphene surfaces. The synthesized NC/Ag nanobelt hybrid materials were subsequently used to fabricate the highly conductive fibres (>1000S/cm) that can function as a conformable electrode and highly tolerant strain sensor, as well as a highly conductive and robust paper (>10000S/cm after thermal treatment).