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In this paper, a new method using an ammonia–urea system was proposed to prepare cellulose aerogels from coir fibers as the starting material for non-ordered porous nitrogen-doped carbon aerogels. Direct pyrolysis of the as-prepared carbon aerogels has successfully produced nitrogen-doped carbon aerogels using the cellulose aerogel derived from the nitrogen-rich coir fibers. The as-prepared carbon aerogel inherits the three-dimensional nonordered porous network of the cellulose aerogel, maintaining its high specific surface area (SSA) and the large pore volume. In addition, the honeycomb-like structure of internal pores in individual fibers could also be maintained, and the pores are even larger than those of the corresponding cellulose aerogel. In the ammonia–urea system, ammonia not only served as an agent to assist the cellulose dissolution but also played an important role in exfoliating the carbon …