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The construction of atomically-precise carbon nanostructures holds promisefor developing novel materials for scientific study and nanotechnologyapplications. Here we show that graphene origami is an efficient way to convertgraphene into atomically-precise, complex, and novel nanostructures. Byscanning-tunneling-microscope manipulation at low temperature, we repeatedlyfold and unfold graphene nanoislands (GNIs) along arbitrarily chosen direction.A bilayer graphene stack featuring a tunable twist angle and a tubular edgeconnection between the layers are formed. Folding single-crystal GNIs createstubular edges with specified chirality and one-dimensional electronic featuressimilar to those of carbon nanotubes, while folding bi-crystal GNIs createswell-defined intramolecular junctions. Both origami structural models andelectronic band structures were computed to complement analysis of theexperimental results. The present atomically-precise graphene origami providesa platform for constructing novel carbon nanostructures with engineered quantumproperties and ultimately quantum machines.

Atomically-Precise, Custom-Design Origami Graphene Nanostructures