The content of plutonium isotopes in high burnup pressurized water reactor fuel samples was examined using both alpha spectrometry and mass spectrometry after anion exchange separation. The measured values were compared with results calculated by the ORIGEN-2 code. On average, the ratios (m/c) of the measured values (m) over the calculated values (c) were 1.22±0.16 for 238 Pu, 1.02±0.14 for 239 Pu, 1.08±0.06 for 240 Pu, 1.06±0.16 for 241 Pu, and 1.13±0.08 for 242 Pu. Using the Pu data obtained in this work, correlations were derived between the alpha activity ratios of 238 Pu/( 239 Pu+ 240 Pu), the alpha specific activities of Pu, and the atom % abundances of the Pu isotopes. Using these correlations, the atom % abundances of the plutonium isotopes in the target samples were calculated. These calculated results agreed within a range from 2 to 8% of the experimentally derived values according to the isotopes of plutonium.