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The urgent requirement of materials with superior electromagnetic shielding properties has been aroused for alleviating electromagnetic pollution. Now, some natural materials such as silkworm cocoon, walnut shell, and so on are gradually used to prepare the electromagnetic interference shielding composites. However, loofah sponges with unique and inherent 3D hierarchical porous structure, which could be obtained from food waste and the wilted loofah, are ignored. In this work, loofah sponges were modified by NaOH and H2O2. Then the carbonized modified Loofah/Ni nanoparticles/Graphene composites were prepared by immersion and thermal reduction. Meanwhile, the composites had inherited advantages from natural materials such as low density, porous structure and eco-friendly. As the result of loading of Ni nanoparticles and graphene on the loofah, the outstanding performance was achieved that the shielding effectiveness was raised to 57 dB, and the specific shielding effectiveness was raised to 616.8 dB cm3/g. This result demonstrated that composites materials based on natural loofah sponges show tremendous potential for electromagnetic shielding.