In the current study, the gamma-radiation-shielding characteristics of novel gypsum–lime–waste marble-based mortars reinforced with micro-PbO and nano-PbO powders were investigated. In total, seven mortar groups, including a control mortar (named GLM), were prepared. The other groups contained10, 20, and 30 wt.% of both micro-PbO and nano-PbO as a waste marble replacement. This study aimed to explore the effect of particle size and concentrations of PbO powders on the γ-ray-shielding capability of GLM mortars. For this purpose, an HPGe detector and five standard radioactive point sources (241Am, 133Ba, 137Cs, 60Co, and 152Eu) were employed to measure different shielding parameters, including the linear attenuation coefficient (μ), mass attenuation coefficient (μm), mean free path (MFP), half-value layer (HVL), and tenth-value layer (TVL), for the prepared samples in the energy range between 59.53 keV to 1408.01 keV. On the basis of μm values, other significant shielding parameters such as effective atomic number (Zeff), effective electron density (Neff), equivalent atomic number (Zeq), and exposure buildup factor (EBF) were also computed to explore the potential usage of the proposed mortars as radiation protective materials. The results reported that the smallest HVL, TVL, and MPF, as well as the largest attenuation values, were obtained for mortars reinforced by nano-PbO compared to those containing micro-PbO. It can be concluded from the results that the mortar samples containing nano-PbO had a remarkably improved gamma-radiation-shielding ability. Thus, these mortars can be used for radiation shielding on walls in nuclear facilities to reduce the transmitted radiation dose.