The hydrothermal synthesis of nitrogen-doped monolithic carbon aerogels derived from sustainable precursors (i.e.D-glucose and ovalbumin) is presented. The protein acts as nitrogen donor and surface stabilizing agent in this saccharide hydrothermal carbonization, to generate high surface area aerogels (>240 m2g−1) composed of functional continuous large diameter mesopores with excellent hierarchical transport architecture. Post-carbonization treatment controls surface chemistry (e.g. C or N condensation), facilitating tuneable physicochemical properties on a unique continuous 3D carbonaceous pore structure. This highly flexible synthesis lays the basis for the development of a new generation of sustainable (heteroatom-doped) porous carbon aerogels suitable for a range of high value applications.