Improving mortar shielding properties to preserve environmental and human safety in radiation facilities is essential. Conventional cement mortars, composed of cement, water, and lime aggregate, are crucial for radiation shielding. Using recycled aggregates to produce new mortar and concrete compositions has attracted the attention of several researchers. In the current study, waste marble and iron slag as aggregates are used to create novel cement mortar compositions to study the aggregate’s impact on the radiation attenuation capability of the mortar. Three mortar groups, including a control mortar (CM-Ctrl), were prepared based on cement and waste marble. The other two groups (CM-MIS, CM-NIS), contained 25% iron slag at different particle sizes as a replacement for a waste marble. The study aims to compare iron slag in their micro and nano sizes to discuss the effect of particle size on the mortar radiation capability. For this purpose, the NaI scintillation detector and radioactive point sources (241Am, 133Ba, 137Cs, 60Co, and 152Eu) were utilized to measure several shielding parameters, such as the linear attenuation coefficient (LAC), mass attenuation coefficient (MAC), half-value layer (HVL), tenth-value layer (TVL), and mean free path (MFP), for the produced mortars at different photon energies. Furthermore, the transmission electron microscope (TEM) is used to measure the particle size of the aggregates. In addition, a scanning electron microscope (SEM) is utilized to acquire the cross-section morphologies of the prepared mortars. According to our findings, mortars prepared with nano-iron slag and waste marble offered superior shielding capabilities than mortars containing natural sand or fine crushed stone. The nano iron slag mortar can be utilized in place of typical sand mortar for applications as rendering or plastering materials for building medical diagnostic and CT scanner rooms, due to its improved shielding abilities.