The MCNP-5 code was utilized to simulate the mass attenuation coefficient (MAC) of a novel series of chalcogenide spinels called XCr2Te4 (where X represents Co, Fe, and Cu). Following preparation through the conventional solid-state reaction method, the samples exhibited densities ranging from 6.42 to 7.04 g cm−3. By comparing the obtained results with the XCOM data, we observed a significant correlation with a relative difference of 0–1.93%. The accuracy of the simulated data was further confirmed by performing the Kolmogorov-Smirnov test. Based on the calculated MAC, we derived several radiation parameters. Finally, these derived results were compared to previously published data for evaluation. These parameters showed the superiority of the sample containing Co (CT-Co) over other samples on gamma and neutron shielding properties. The results illustrate the ability of studied samples to absorb most gamma-ray photons within low energies, which suggests the potential for applying radiation shielding fields.