This work is an attempt to employ the electric arc furnace (EAF) slag as a by-product material to develop an alternative and environmentally friendly material for gamma-radiation protection applications such as in medical and industrial areas. For this purpose, different concentrations of micro-sized EAF slag (0, 20, 40, 60, 80, 100, 500, and 800 phr) were incorporated as fillers in the natural rubber (NR) matrix to produce the shielding composites. In addition, nano-sized EAF slag particles were prepared by using a high-energy ball milling technique to investigate the effect of particle size on the gamma-radiation shielding properties. The synthesized micro and nano EAF/NR composites were tested as protective materials against gamma-radiation by employing NaI(Tl) scintillation detector and standard radioactive point sources (152Eu, 137Cs, 133Ba, and 60Co). Different shielding parameters such as linear and mass attenuation coefficient, half value layer (HVL), tenth value layer, mean free path, effective atomic number (Zeff), and effective electron density (Neff) were determined to assess the radiation shielding capability of the EAF/NR composites. Furthermore, equivalent atomic number (Zeq) and the exposure buildup factor values for photon energy in the range from 0.015 to 15 MeV were also computed by Geometric Progression method. The experimental results of micro EAF/NR composites showed that at 121.78 keV, EAF0 composite (without EAF slag content) had the lowest μ value of 0.1695 cm−1, while the EAF800 composite (which was loaded with 800 phr of micro EAF slag) had the highest μ value of 0.2939 cm−1 at the same energy, which in turn decreases the HVL from 4.09 to 2.36 cm, respectively. Therefore, increasing the filler weight fractions of EAF slag in the NR matrix, increases the shielding properties of the composites. Moreover, the NR composite reinforced with 800 phr of nano EAF slag has better gamma-radiation shielding efficiency compared to that filled with 800 phr of micro EAF slag. The success of this work was to prepare a flexible, lightweight, low-cost, and lead-free material with better shielding capability.