Correspondence to: hjgao@iphy.ac.cn, sxdu@iphy.ac.cn †These authors contributed equally to this work.The construction of atomically-precise carbon nanostructures holds promise for developing novel materials for scientific study and nanotechnology applications. Here we show that graphene origami is an efficient way to convert graphene into atomically-precise, complex, and novel nanostructures. By scanning-tunneling-microscope manipulation at low temperature, we repeatedly fold and unfold graphene nanoislands (GNIs) along arbitrarily chosen direction. A bilayer graphene stack featuring a tunable twist angle and a tubular edge connection between the layers are formed. Folding single-crystal GNIs creates tubular edges with specified chirality and onedimensional electronic features similar to those of carbon nanotubes, while folding bicrystal GNIs creates well-defined intramolecular junctions. Both origami structural models and electronic band structures were computed to complement analysis of the