Molecular-dynamics simulations have been performed to investigate metallic-nanowire (NW) induced spontaneous scrolling of single-layered graphene (SLG) nanostructures. This unique behavior is attributed to the van der Waals attraction between the SLG and NW and theπ-π stacking effect between SLG layers. The scrolling velocity shows a nonlinear dependence on time. Such self-scrolling of SLG is hindered by the surface roughness and especially the oxygen concentration of NW. SLGs with arbitrary sizes and shapes can wrap onto NW to form various configurations. The proposed discoveries eventually provide a powerful way to fabricate nanoscale composite materials and devices and tune their properties.