This study presents a novel metamaterial design for robust ultra-broadband microwave absorption, addressing challenges such as narrow bandwidth, low-frequency bottlenecks, and the need for robustness against oblique and polarized incidence. The design features a 2D/2D assembly of semiconductive metal-organic frameworks (CuHT) and flake-layered carbonyl iron powders (FCIP), resulting in a material with a thickness of just 9.3 mm that achieves significant EMW absorption across a broad frequency range (2 to 40 GHz). The CuHT-FCIP composite exhibits strong magnetoelectric coupling, leading to enhanced EMW loss. The material is encapsulated in an electromagnetic transparent epoxy resin (CuHT-FCIP-EP) to further improve its performance, achieving an effective modulation of the EMW absorption bandwidth. The CuHT-FCIP-EP metamaterial is then integrated into a 3D metamaterial design with a gradient impedance and honeycomb perforation, resulting in an ultra-broadband absorber with excellent performance in terms of bandwidth, thickness, and mechanical strength. This advancement holds promise for developing advanced EMW absorbers with superior performance, suitable for mass production and practical applications.This study presents a novel metamaterial design for robust ultra-broadband microwave absorption, addressing challenges such as narrow bandwidth, low-frequency bottlenecks, and the need for robustness against oblique and polarized incidence. The design features a 2D/2D assembly of semiconductive metal-organic frameworks (CuHT) and flake-layered carbonyl iron powders (FCIP), resulting in a material with a thickness of just 9.3 mm that achieves significant EMW absorption across a broad frequency range (2 to 40 GHz). The CuHT-FCIP composite exhibits strong magnetoelectric coupling, leading to enhanced EMW loss. The material is encapsulated in an electromagnetic transparent epoxy resin (CuHT-FCIP-EP) to further improve its performance, achieving an effective modulation of the EMW absorption bandwidth. The CuHT-FCIP-EP metamaterial is then integrated into a 3D metamaterial design with a gradient impedance and honeycomb perforation, resulting in an ultra-broadband absorber with excellent performance in terms of bandwidth, thickness, and mechanical strength. This advancement holds promise for developing advanced EMW absorbers with superior performance, suitable for mass production and practical applications.