The integration of single wall carbon nanotubes (single wall CNTs or SWCNTs) in large-scale applications is still halted by the lack of control and by the limited understanding of factors influencing growth. [1] In particular, the synthesis of sub-nm semiconducting and metallic SWCNTs has proven to be difficult due to problems associated with catalyst nanoparticle coarsening and the slow kinetics at the lower temperatures and pressures required for their growth. Sub-nm diameter semiconducting SWCNTs exhibit electrical bandgaps greater than 1 eV while their metallic counterparts exhibit bandgaps <0.14 eV, [2] making them ideal for electronic devices. Although significant progress has been made in the past decade toward achieving controlled growth of SWCNTs, [3] factors such as particle/support interactions, particle/tube epitaxy, and kinetics mainly result in the A challenge in the synthesis of single-wall carbon nanotubes (SWCNTs) is the lack of control over the formation and evolution of catalyst nanoparticles and the lack of control over their size or chirality. Here, zeolite MFI nanosheets (MFI-Ns) are used to keep cobalt (Co) nanoparticles stable during prolonged annealing conditions. Environmental transmission electron microscopy (ETEM) shows that the MFI-Ns can influence the size and shape of nanoparticles via particle/ support registry, which leads to the preferential docking of nanoparticles to four or fewer pores and to the regulation of the SWCNT synthesis products. The resulting SWCNT population exhibits a narrow diameter distribution and SWCNTs of nearly all chiral angles, including sub-nm zigzag (ZZ) and near-ZZ tubes. Theoretical simulations reveal that the growth of these unfavorable tubes from unsupported catalysts leads to the rapid encapsulation of catalyst nanoparticles bearing them; their presence in the growth products suggests that the MFI-Ns prevent nanoparticle encapsulation and prologue ZZ and near-ZZ SWCNT growth. These results thus present a path forward for controlling nanoparticle formation and evolution, for achieving size-and shape-selectivity at high temperature, and for controlling SWCNT synthesis.