A 2D/2D coupled MOF/Fe composite metamaterial enables robust ultra-broadband microwave absorption. The study proposes a metamaterial design that addresses challenges in electromagnetic wave (EMW) absorption, including narrow bandwidth, low-frequency bottlenecks, and robustness under oblique and polarized incidence. The absorber features a semiconductive metal-organic framework/iron 2D/2D assembly (CuHT-FCIP) with abundant crystal/crystal heterojunctions and strong magneto-electric coupling networks. This design achieves remarkable EMW absorption across a broad range (2 to 40 GHz) at a thickness of just 9.3 mm. Notably, it maintains stable performance against oblique incidence (within 75°) and polarizations (both transverse electric and transverse magnetic). Furthermore, the absorber demonstrates high specific compressive strength (201.01 MPa·cm³·g⁻¹) and low density (0.89 g·cm⁻³). This advancement holds promise for developing robust EMW absorbers with superior performance. The study explores the use of semiconductive metal-organic frameworks (SC-MOFs) combined with strong magnetic materials to achieve a superior magnetoelectric coupling effect, enhancing EMW absorption capabilities and expanding the effective absorption bandwidth (EAB) when applied in 3D metamaterials. The CuHT-FCIP composite is fabricated by immersing CuHT and FCIP in an ethanol solution and subjecting it to bath sonication. The resulting composite is encapsulated in an electromagnetic transparent epoxy resin (CuHT-FCIP-EP) and integrated into a novel 3D metamaterial design with gradient impedance and honeycomb perforation. The as-prepared CuHT-FCIP-EP metamaterials show robust microwave absorption performance with an ultra-broad EAB from 2 GHz to 40 GHz, ultra-wide oblique adaptability within 75°, and high polarization insensitivity. The material also exhibits excellent mechanical performance, making it suitable for mass production and development of functional ultra-broadband EMW absorbers.A 2D/2D coupled MOF/Fe composite metamaterial enables robust ultra-broadband microwave absorption. The study proposes a metamaterial design that addresses challenges in electromagnetic wave (EMW) absorption, including narrow bandwidth, low-frequency bottlenecks, and robustness under oblique and polarized incidence. The absorber features a semiconductive metal-organic framework/iron 2D/2D assembly (CuHT-FCIP) with abundant crystal/crystal heterojunctions and strong magneto-electric coupling networks. This design achieves remarkable EMW absorption across a broad range (2 to 40 GHz) at a thickness of just 9.3 mm. Notably, it maintains stable performance against oblique incidence (within 75°) and polarizations (both transverse electric and transverse magnetic). Furthermore, the absorber demonstrates high specific compressive strength (201.01 MPa·cm³·g⁻¹) and low density (0.89 g·cm⁻³). This advancement holds promise for developing robust EMW absorbers with superior performance. The study explores the use of semiconductive metal-organic frameworks (SC-MOFs) combined with strong magnetic materials to achieve a superior magnetoelectric coupling effect, enhancing EMW absorption capabilities and expanding the effective absorption bandwidth (EAB) when applied in 3D metamaterials. The CuHT-FCIP composite is fabricated by immersing CuHT and FCIP in an ethanol solution and subjecting it to bath sonication. The resulting composite is encapsulated in an electromagnetic transparent epoxy resin (CuHT-FCIP-EP) and integrated into a novel 3D metamaterial design with gradient impedance and honeycomb perforation. The as-prepared CuHT-FCIP-EP metamaterials show robust microwave absorption performance with an ultra-broad EAB from 2 GHz to 40 GHz, ultra-wide oblique adaptability within 75°, and high polarization insensitivity. The material also exhibits excellent mechanical performance, making it suitable for mass production and development of functional ultra-broadband EMW absorbers.