To support the development of Sodium-cooled Fast Reactors (SFRs) of Generation IV nuclear energy systems and to study the use of the TRIPOLI-4® Monte Carlo code and the JEFF-3.1.1 nuclear data library on the core neutronics of large fast neutron reactors, in this work two recent Organisation for Economic Co-operation and Development/Nuclear Energy Agency (OECD/NEA) computational benchmarks of two 3600-MW(thermal) SFRs were analyzed with the continuous-energy TRIPOLI-4 code. Both a mixed oxide [(U,Pu)O2] core and a carbide [(U,Pu)C] core were investigated. Under two different fast neutron spectra, the reactor physics parameters—Keff, βeff (effective delayed neutron fraction), sodium void worth, Doppler constant, control rod worth, and core power distribution—were calculated for the beginning of equilibrium cycle condition. Both the pin-by-pin heterogeneous and fuel assembly–level homogeneous calculation models were applied in the whole-core simulation in order to evaluate their impact on the calculation results of SFR reactor physics parameters. The ENDF/B-VII.0 data library from the evaluation was also used with TRIPOLI-4 to study its impact on the SFR core reactivity and the boron carbide control rod worth. Using the mesh tally option, the energy deposition tally, and the upgraded display tool of TRIPOLI-4, radial power distribution and core power maps of the two cores were calculated and compared.