Lead-free polymer composite shields are used in diagnostic radiology to protect patients from unnecessary radiation exposure. This study aimed to examine and introduce the radiation-shielding properties of single- and multi-metal nanoparticle (NP)-based composites containing Bi, W, and Sn using Geant4, MCNPX, and XCom for radiological applications. The mass attenuation coefficients and effective atomic numbers of single- and multi-metal NP-loaded polymer composites were calculated using the Geant4 and MCNPX simulation codes for X-ray energies of 20-140keV. The nano-sized fillers inside the polydimethylsiloxane (PDMS:C2H6SiO) matrix included W (K = 69.5keV), Bi (K = 90.5keV), and Sn (K = 29.20keV). For single-metal shields, one filler was used, while in multi-metal shields, two fillers were required. The MCNPX and Geant4 simulation results were compared with the XCom results. The multi-metal NP composites exhibited higher attenuation over a larger energy range owing to their attenuation windows. In addition, Bi2O3 + WO3 NPs showed a 39% higher attenuation at 100-140keV, and that of Bi2O3 + SnO2 NPs was higher at 40-60keV. Meanwhile, the WO3 + SnO2 NPs exhibited lower attenuation. The difference between the results obtained using Geant4 and XCom was less than 2%, because these codes have similar simulation structures. The results show that the shielding performance of the Bi2O3 + WO3 filler is better than that of the other single- and multi-metal fillers. In addition, it was found that the Geant4 code was more accurate for simulating radiation composites.