The study covers shielding properties of three promising lead-free XCr2Se4 alloys, where X represents Mn, Cu, or Ag, across a spectrum of energies between 0.02 MeV and 15 MeV. MCNP4C was employed to simulate the mass attenuation coefficient (MAC) for the three selected alloys. After being prepared using the conventional solid-state reaction method, the samples displayed densities ranging from 5.45 g cm−3to 6.22 g cm−3. The simulated results obtained from the MCNP4C are then benchmarked with data obtained using different software such as Phy-X, Py-MLBUF, EPIXS, and GRASP. Upon comparing the acquired results with the Phy-X data, a notable correlation was observed with a relative difference ranging from 0.11% to 8.57%. The accuracy of the simulated data was additionally validated through the Kolmogorov-Smirnov test. From the simulated MAC, different ionizing radiation shielding properties including linear attenuation coefficient (LAC), half-value layer (HVL), mean-free path (MFP), transmission factor (TF), radiation protection efficiency (RPE), and fast neutron removal cross section (FNRCS) were calculated to provide a comprehensive analysis of the samples' efficacy in dealing with different types of radiation. The LAC for neutrons at different energies is also examined. HVL analysis indicates the radiation-blocking capacity of the samples. The TF shows the alloys’ ability to either permit or restrain the transfer of radiation. Additionally, RPE and FNRCS give indication of the shielding potential of the studied samples. This study is important for nuclear physicians and researchers and serves as useful data for the development of superior shielding materials.