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Attribute to their unique structure-dependent properties, single-walled carbon nanotubes (SWNTs) have great potentials in many fields, for example, electronics,sensors, and energy devices.The structure-controlled preparation of SWNTs is a crucial issue for their advanced applications and has been a great challenge for about two decades.According to the generally accepted vapor-liquid-solid (VLS) mechanism of SWNT growth in a chemical vapor deposition (CVD) process, catalysts play essential roles in carbon feedstock decomposition, SWNT nucleation and growth.By careful design on the composition and structure of catalyst nanoparticles, we explored the property and structure controlled synthesis of SWNTs.Pure semiconducting SWNTs and chirality pure SWNTs were prepared via such methodology.