The commercialization of carbon nanotubes (CNTs) depends on rapid development in precise structure control and morphological assembly technology. In article number 2109401,Weizhong Qian, Fei Wei, and co-workers summarize the catalytic growth mechanism of defect-free CNTs. The template-assisted morphological assembly is subsequently introduced as an efficient route towards their mass production. Finally, more cutting-edge applications are presented with potential breakthroughs in fibers, energy, and electronics.