The energy group structure of a multi-group cross section library matched with a deterministic method has a significant influence on shielding calculation. The complex resonance cross section of Fe-56 has a significant influence on accuracy with different energy group structures when processing multi-group cross section data. In this study, in order to more accurately test the influence of the iron resonance phenomenon on shielding calculations, this group structure is modified by the 199-group with 69 points interpolated into its group boundaries at an energy range from 1.1 keV to 3.1164 MeV. The new 269-group library is then tested with selected SINBAD iron sphere benchmarks and compared with the results of 199-group, 299-group, and 172-group libraries and measurements. Upon analysis, it is shown that the resonance of Fe-56 has a great influence on the accuracy of the calculated leakage. Further, it is noted that the finer the energy group division, the greater the calculated leakage fluctuation, and the deeper the neutron passes through the iron sphere, the larger the calculated leakage fluctuation. This study and its leakage results may provide a good reference for the development of new multi-group structures for present and future shielding design.