Well-known hard-template methods for nitrogen (N)-doped chiral carbon nanomaterials require complicated construction and removal of the template, high-temperature pyrolysis, harsh chemical treatments, and additional N-doping processes. If naturally occurring chiral nematic chitin nanostructures [(C8H13NO5)(n)] in exoskeletons were wholly transformed into an N-doped carbon, this would be an efficient and sustainable method to obtain a useful chiral nanomaterial. Here, a simple, sacrificial-template-free, and environmentally mild method was developed to produce an N-doped chiral nematic carbon-sheath nanofibril hydrogel with a surface area >300 m(2) g(-1) and enantioselective properties from renewable chitin biomass. Calcium-saturated methanol physically exfoliated bulk chitin and produced a chiral nematic nanofibril hydrogel. Hydrothermal treatment of the chiral chitin hydrogel at 190 degrees C produced an N-doped chiral carbon-sheath nanofibril hydrogel without N-doping. This material preferentially adsorbed d-lactic acid over l-lactic acid and produced 16.3 % enantiomeric excess of l-lactic acid from a racemic mixture.