This research investigates the impact of incorporating low-cost MnFe2O4 spinel nanoparticles (MF-NPs) at varying concentrations (0.5, 1, and 2 mass%) on the mechanical and physical properties of blended cement pastes. These pastes were produced by replacing different proportions (5, 10, and 15 mass%) of ordinary Portland cement (OPC) with activated alumina sludge waste (AAS), to promote sustainability. Also, the research examined the gamma radiation shielding effectiveness of certain hardened composites against a 137Cs gamma radiation source with an energy of 661.64 keV using a NaI (Tl) detector (Oxford Model) with 3″ × 3″, amplifier and 16 k multi-channel analyzer. The linear attenuation coefficient (LAC) of all the studded samples were calculated theoretically using a Monte Carlo code MCNP-5 code. The gamma radiation shielding properties were analyzed in depth using a Monte Carlo code MCNP-5 simulation model. The theoretical and experimental results for LAC were found to be in complete agreement. Phy-X/PSD software was applied to estimate the mass attenuation coefficient (MAC) for gamma radiation at various energies, as well as the effective atomic number (Zeff), mean free path (MFP), half-value layer (HVL), and tenth-value layer (TVL). The findings demonstrated that the addition of 0.5% MnFe2O4 nanoparticles (MF-NPs) to blended cement pastes exhibited the best physical and mechanical characteristics, as well as the most effective gamma radiation shielding.