From　a　material　design　perspective,　the　incorporation　of　Fe3O4@carbon　nanotube　(Fe3O4@CNT)　hybrids　is　an　effective　approach　for　reconciling　the　contradictions　of　high　shielding　and　low　reflection　coefficients,　enabling　the　fabrication　of　green　shielding　materials　and　reducing　the　secondary　electromagnetic　wave　pollution.　However,　the　installation　of　Fe3O4　nanoparticles　on　nonmodified　and　nondestructive　CNT　walls　remains　a　formidable　challenge.　Herein,　a　novel　strategy　for　fabricating　the　above-mentioned　Fe3O4@CNTs　and　subsequently　assembling　segregated　Fe3O4@CNT　networks　in　natural　rubber　(NR)　matrices　is　proposed.　The　advanced　and　unique　structure,　magnetism,　and　lossless　conductivity　endow　the　as-obtained　Fe3O4@CNT/NR　with　a　shielding　effectiveness　(SE)　of　63.8 dB　and　a　low　reflection　coefficient　of　0.24,　which　indicates　a　prominent　green-shielding　capability　that　surpasses　those　of　previously　reported　green-shielding　materials.　Moreover,　the　specific　SE　reaches　531 dB　cm−1,　exceeding　that　of　those　of　previously　reported　carbon/polymer　composites.　Meanwhile,　the　outstanding　conductivity　enables　the　composite　to　reach　a　saturation　temperature　of　≈95 °C　at　a　driving　voltage　of　1.5 V　with　long-term　stability.　Therefore,　the　as-fabricated　Fe3O4@CNT/rubber　composites　represent　an　important　development　in　green-shielding　materials　that　are　applied　in　cold　environment.　©　2023　Wiley-VCH　GmbH.