Carbon nanotubes (CNTs) have captivated scientists for over 25 years due to their unusual combination of mechanical and solid-state properties. Their potential applications span a wide range of fields including biomedical technologies, electronics, optics, sensors, and strong, lightweight composites. Despite their potential and demonstration of application-level performance in the past decade, CNTs have not achieved widespread adoption. CNT manufacturing remains small-scale with high production costs, a critical barrier to broader utilization. The most common techniques for growing high-purity and crystalline CNTs are based on chemical vapor deposition (CVD); in principle, they are simple methods and have the potential for bulk production scaling. One such method, floating catalyst CVD (FCCVD), has been employed successfully to grow both single-walled CNTs (SWCNTs) and multi-walled CNTs (MWCNTs). However, multiple dynamic processes occur within the FCCVD reactor, which complicates reactor understanding and makes production control challenging. With few, recent exceptions, the FCCVD system has been treated as a black box; however, increasing synthesis efficiency and scale requires a deeper understanding of the coupled chemical and transport processes occurring. In this thesis, a perspective on the climate mitigation potential for large-scale CNT production (Chapter 1) is presented followed by a review of the FCCVD literature (Chapter 2). In the final chapters of the thesis, in-depth materials and process analyses are presented which will have implications for large-scale CNT production.