The research and development of functional nanostructured carbons (FNCs) or FNC-based catalysts for heterogeneous catalysis is a highly dynamic and important topic in academia and industry because FNCs show integrated advantages: accessible pore system, regular pore structure, controlled bulk composition and surface chemistry, rapid ionic and electron mobility, etc as compared to their conventional analogs. Rather than a detailed treatise into every aspects of FNCs, this short review attempts to highlight some critical and important issues of a series of FNCs based on some representative reactions: (1) the pathways in rational fabrication of the structure and chemistry controlled FNCs, (2) the strategies to make the most of structural merits in design of high-performance catalysts based on FNCs, (3) the possible roles of textural parameters and surface heterogeneities of FNCs on catalytic behaviors. Finally, the challenges in the design of more tailored FNCs and FNC-based catalysts are pointed out, and the need of advanced characterizations and computational predication for in-depth understanding of carbon physics and chemistry of FNCs as well as catalysis mechanisms are suggested.