Abstract: Compared with pristine monolayer graphene, graphene nanostructures (GNSs), that is, low-dimensional sp² -based nanocarbons, exhibit more interesting and novel properties which may be applied to construct graphene-based nanodevices. The electronic properties of these nanostructures have been predicted to depend sensitively on the atomic configuration parameters such as shape, size, edges, vacancies and adatoms. Therefore, it is crucial to construct welldefined, atomically- precise GNSs, and to study their unique properties. We have conducted a series of experiments to fabricate high- quality GNSs with special configurations on various substrates using precisely-controlled methods and low-temperature, strong-magnetic-field scanning tunneling microscopy. Through manipulation of the latter, we have constructed atomically-precise, custom-designed graphene nanostructure origami. These results provide new platforms for constructing carbon nanostructures with engineered quantum properties.