We report a novel phenomenon in carbon nanotube growth that results in a new carbon nanotube morphology. A carbon nanotube grown via metal nanoparticle-catalyzed chemical vapor deposition splits into two flattened nanotubes during growth and the two flattened nanotubes merge to form a ring of carbon nanotube/nanoribbon. This novel process is revealed with transmission electron microscopy observations of the carbon nanostructures. We propose that the splitting-and-joining process involves only one metal catalyst nanoparticle and a self-folding mechanism that we have named the origami mechanism to explain the process and the formation of nanoribbons and nanotetrahedra.Branching in carbon nanotube (CNT) growth was first reported by Zhou and Seraphin 1 , where CNTs grown by carbon arc-discharge appeared to have horn-like projections in three directions. This novel phenomenon aroused interest in the fundamental aspects of catalytic CNT growth and opened up new possibilities of CNT application to various devices and to nanowiring. After this discovery, many groups reported the formation of Y-branched (Y-junction) and multi-branched CNTs prepared using various methods. The most standard methods employed for the fabrication of branched CNTs are pyrolysis and catalytic chemical vapor deposition (CVD) 2-11 . Four different formation processes for branched CNTs have been identified in these studies. (i) Several CNTs can grow simultaneously from a catalyst metal nanoparticle or sequentially. (ii) A catalyst metal nanoparticle moves back into the formed CNT and a branch is formed. (iii) A catalyst metal nanoparticle is broken into fragments and each forms a branch. (iv) Catalyst nanoparticles are attached onto the surface of a trunk CNT and each catalyst particle forms a branch. There are two other methods for the fabrication of branched CNTs; welding 12-15 and the use of templates [16][17][18] . These two methods/modes are not directly related to the fundamental aspects of metal-nanoparticle-catalyzed CNT growth; therefore, they are not discussed in detail here.In the metal-nanoparticle-catalyzed growth by these four modes, branches are always formed from the CNT trunk. Only one exception can occur when the catalyst metal nanoparticle of a CNT makes arbitrary contact with another distinct CNT or catalyst metal nanoparticle and these two CNTs then merge into one 15 . In this paper, we report a novel phenomenon in the metal-nanoparticle-catalyzed growth of multi-walled CNTs, where a CNT grown from a catalyst metal nanoparticle splits into two flattened CNTs (nanoribbons) that continue to grow simultaneously from the metal nanoparticle, followed by joining of the two nanoribbons to form a single tubular or flattened CNT. This results in the formation of a closed loop. The origin of CNT splitting is attributed to a mechanism we have named the origami mechanism, in which a CNT that is expelled from a metal nanoparticle is forced to be flattened in two opposing directions 19,20 . Figure 1 shows transmission electron microscopy (T...