This study deals with the preparation of magnetite nanoparticles (NPs) via a coprecipitation method using several precipitation bases: binary precipitator (NH4OH), mono precipitator (NaOH), and weak precipitator (Ca(OH)2). The prepared magnetite NPs were identified using X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM), energy-dispersive X-ray (EDX) analysis, surface area analysis, magnetic properties, Fourier-transformed infrared spectra (FT-IR), and ultra-violet UV–visible spectra. As a result, the phases of the produced magnetite NPs were unaffected by the use of various bases, but their crystallite sizes were affected. It was found that the binary base provided the smallest crystallite size, the mono base provided an average size, and the weak base provided the largest crystallite size. The UV–visible absorption spectroscopy investigation revealed that the absorption and the energy gap rose with a reduction in nanoparticle size. The prepared magnetite NPs were used to manufacture polymeric-based nanocomposites employed as protective shields from low-energy X-rays that are light in weight. These samples were identified using XRD, atomic force microscopy (AFM), and FT-IR spectroscopy. The crystallite size was slightly larger than it was in the case of magnetite NPs. This is consistent with the results of AFM. The interference between the two phases was observed in the results of the FT-IR spectra. The effects of the size of the magnetite NPs on the attenuation tests, linear attenuation coefficient, mass attenuation coefficient, half-value layer, and mean free path were investigated. The results showed that the efficiency of using manufactured shields increases with the decrease in the NPs size of the magnetite used as a reinforcement phase for a range of low operating voltages.