<div>This thesis describes using a series of polyacrylonitrile (PAN)-based architectures as precursors for heteroatom-doped nanocarbons. Chapter 1 is an introduction chapter, focusing on fundamental knowledge and the state-of-the-art of research in the nanocarbon area. Chapters 2-8 demonstrate my research work during my Ph.D. career in Carnegie Mellon University. Among them chapters</div><div>2-4 focus on N-doped nanocarbons, while chapters 5-7 introduce co-doped nanocarbon systems, namely N/B, N/S, and N/Fe co-doped nanocarbons. Chapter 2 is a continuation of previous work using poly(n-butyl acrylate)-b-polyacrylonitrile linear block copolymer as carbon precursors. Here, we used supplemental activators and reducing agents (SARA) ATRP to achieve more precisely</div><div>controlled polymer precursors and gained deeper insight about the produced porosity in nanocarbons. Chapter 3 introduces using novel PAN-b-PBA bottlebrushes as carbon precursors. Chapter 4 demonstrates a novel core/shell particle-based strategy to produce porous carbon spheres,</div><div>and compare its performance with carbon monolith in different applications. Chapter 5 extends the CTNC technique to N/S co-doped nanocarbon by establishing a new PAN stabilization strategy using sulfur. Chapter 6 extends the CTNC technique to N/B co-doped nanocarbon by using a boron-containing monomer. Chapter 7 focuses on using CTNC as a base material and doping it</div><div>with Fe for platinum group metal free (PGM-Free) fuel cells. Chapter 8 demonstrates using different PAN-based polymers to wrap carbon nanotubes with controlled polymer thickness. Finally, a summary with outlook on future directions is provided in Chapter 9. Appendices</div><div>summarized all published papers during my Ph.D. study.</div>