Carbon nanotubes (CNTs) are nanomaterials that have attracted great research interest because of their unique properties and promising applications. The controllable synthesis of CNTs is a precondition for their broad application. In this review, we consider nanoscale process engineering and assess recent progress in the mass production of ultra-long, inexpensive CNTs with good alignment as well as tunability in wall number and diameter for fundamental and engineering science applications across multiple scales. Cutting-edge nanoscale process engineering research in the areas of physics, chemistry, materials, engineering, ecology, and social science will allow us to obtain high added value and multi-functional advanced CNTs. The synthesis of CNTs with controllable chirality, good-alignment, and predetermined sizes and lengths still presents great challenges. Through multidisciplinary scientific research, advanced CNT-based materials will promote the development of a sustainable society.