During reactor operations and fuel bum up, some isotopic abundances change due to nuclear reactions and provide sensitive indicators of neutron fluence and fuel burnup. Secondary ion mass spectrometry (SIMS) analysis has been used to measure isotope ratios of selected impurity elements in irradiated nuclear reactor graphite. Direct SIMS measurements were made in graphite samples, following shaping and surface cleaning. Models predicting local fuel burnup based on isotopic measurements of B and Li isotopes by SIMS agreed well with U and Pu isotopic measurements obtained by thermal ionization mass spectrometry (TIMS). (c) 2006 Elsevier B.V. All rights reserved.