The synergistic effects of a hybrid nanocomposite (Fe3O4@NrGO) and their influence on electromagnetic pollution shielding (EMI SE) were explored. This is a current concern where the impacts need to be fully clarified and assertively addressed. Thus, the main focus of the paper was based on the physical and mechanical properties of porosity, surface area, flexibility and, mainly, electrical conductivity of the graphene aerogels, which do not require the use of a binder and are of great interest for the EMI SE area. The precursors (rGO, NrGO and Fe3O4), as well as the nanocomposite, underwent thorough structural characterisation to understand their nature. Characteristic bands of C-N/C=N bonds and a content of 8.03 at% N were identified, with a high N:O ratio of 1.31, indicating efficient doping of the conductive matrix. The aerogel NrGO phase, with a quality of just 5 layers, and the Fe3O4 phase, with domains around 5 nm, were confirmed, as well as the superposition of the signals in the Fe3O4@NrGO pattern. Electron microscopy images and elemental map also demonstrated the efficient distribution of Fe3O4 in the matrix and its porous appearance. Thus, leveraging the advantages of aerogel, extremely light ultra-thin pellets measuring 0.1 mm and weighing 10 mg were produced. The high nitrogen doping of the graphene network, the presence of magnetic nanoparticles, as well as the high surface area and porosity achieved in the production of the nanocomposite, were responsible for high specific shielding effectiveness of 2730 dB · cm−1 at 10.7 GHz and an average in the X-band of 1590 dB · cm−1. Thus, the improved and synergistic mechanisms highlighted the promising advantages of using these highly porous doped materials, demonstrating that the Fe3O4@NrGO hybrid presents high value for investigations in the application of EMI SE. Display omitted •The Fe3O4@NrGO hybrid nanocomposite presented a synergistic contribution to EMI SE.•The properties of aerogel allowed to obtain light, thin and binder-free pellets.•The specific EMI SE was higher than those reported for graphene-based materials.