The structural relaxation of nanographite ball‐milled in argon atmosphere and stored in evacuated ampoules, has been studied by monitoring the evolution of the Raman spectra. Reduction of some Raman bands associated with “in‐plane” structural defects, such as vacancies, dislocations or grain boundaries, and those associated with “out‐of‐plane” defects, such as stacking faults, is accompanied by the rise of new bands around 1180 and 2000 cm–1. The development of these bands is suppressed in nanographite samples exposed to a flux of pure anhydrous hydrogen. (© 2008 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)