The　exploitation　of　carbon　nanotube　(CNT)　and　metal-organic　framework　(MOF)　composite　materials　has　been　highly　desirable　in　a　number　of　applications.　However,　the　construction　of　high　dispersibility　and　stability　CNT/MOF　complex　structures　is　still　an　enormous　challenge.　Herein,　a　novel　assembly　method　is　established　for　the　construction　of　a　CNT/Ni-MOF　(0.1　CNT/MOF,　0.2　CNT/MOF,　0.3　CNT/MOF)　interpenetrated　structure　by　a　solvothermal　process.　The　MOFs　can　be　robustly　anchored　on　the　surface　of　CNTs.　Through　a　series　of　characterizations,　the　MOF　can　be　comfortably　integrated　into　the　CNT　fibers,　which　exhibits　the　enhancement　of　carrier　mobility　and　fluorescence　properties.　The　microwave　absorption　properties　of　the　CNT/MOF　are　explored　by　a　vector　network　analyzer.　The　0.1　CNT/MOF　has　a　maximum　absorption　of　-9.2　dB　at　18　GHz　with　a　thickness　of　5　mm,　while　the　0.2　CNT/MOF　has　a　maximum　absorption　of　-24.32　dB　at　4.5　GHz　with　a　thickness　of　5　mm,　a　performance　maximum.　Therefore,　the　0.2　CNT/MOF　structures　are　potential　candidates　to　ameliorate　the　microwave　absorption　properties.　©　2020　IOP　Publishing　Ltd.