This work examines the influence of iron oxide nanoparticles (Fe 3O 4 NPs) on neutron and gamma-ray radiation shielding characteristics of Portland cement paste. Experimental evaluations were supplemented with theoretical studies using NXCom program. Portland cement pastes with 5, 10, 15, 20, and 30 wt% of nanomagnetite cement replacement were produced. Moreover, rheological, early strength development, compressive strength, and mercury intrusion porosimetry (MIP) tests were performed. The results showed that increasing the amount of Fe 3O 4 NPs in a mix leads to a gradual increment in measured viscosity and yield stress. High nano-Fe 3O 4 content substantially impeded the early strength development process and led to a decrement in the 7- and 28-day compressive strength of cement paste. The MIP studies exhibited a gradual increment in total porosity, and average pore volume, as nano-Fe 3O 4 content was increased. All the macroscopic cross-sections of slow, fast and thermal neutrons constantly increased as a result of the addition of magnetite nanoparticles, with their variations being markedly linear. Similarly, gamma attenuation test results indicated that the addition of Fe 3O 4 powder enhances the shielding capability of paste in the energy range of interest (0.08–2.614 MeV). In conclusion, Fe 3O 4 nanoparticles can be successfully used in producing lead-free cementitious composites with improved gamma-ray and neutron shielding properties. However, certain drawbacks related to an increment in matrix porosity and thus a decrement in mechanical performance should be taken into account.