In this study, radioactivity of Cs-134, Cs-137, and Eu-154, which are gamma-emitting nuclides among fission products of spent fuel, was analyzed as a tool to measure the burnup of spent fuel nondestructively. This nuclide has a unique gamma-ray energy, allowing the amount of the isotope to be estimated based on the intensity of the gamma-ray at a specific energy. The SCALE 6.2 ORIGAMI (ORIGen AsseMbly Isotopics) module and the latest ORIGEN-arp library were used for computational analysis. The spent fuel samples were selected as WH14×14 with an enrichment of 1.5~5.0wt%, a burnup of 10~60 GWD/MTU, and a cooling time of 0~40 years. The analysis results were benchmarked using SFCOMPO experimental data provided by OECD/ NEA, including isotope inventory and uncertainty measured by destructive radiochemical analysis, fuel assembly design data required for benchmark model development, reactor design information, and operating history information. 16 similar spent fuels were selected from SFCOMPO data and the calculation results of Cs-134, Cs-137, and Eu-154 were compared. The average error of the Cs-134 radioactivity calculation result was 2.81%, and the maximum error was 6.70%. The average errors of Cs-137 and Eu-154 were 2.42% and 4.95%, respectively, and the maximum errors were 5.40% and 14.91%, respectively.