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Electrospun nanofibrous mats are ideal substrates for metalorganic frameworks (MOFs) crystal deposition because of their specific structural parameters and chemical tenability. In this work, we utilized organic-inorganic hybrid electrospun fibrous mats as support material to study the deposition of various MOF particles. HKUST-1 and MIL-53(Al) were produced through solvothermal method, while ZIF-8 and MIL-88B(Fe) were prepared using microwave-induced heating method. The synthesis procedure for both methods were simple and effective because the hybrid nanofibrous mats showed considerable affinity to MOF particles and could be used without additional modifications. The obtained MOF composites exhibited effective incorporation between MOF particles and the porous substrates. MIL-53(Al) composite was applied as fibrous sorbent and showed enhanced adsorption capacity and removal rate, as well as easier operation, compared with thepowdered sample. Moreover, MIL-53(Al) composite was easier to be regenerated compared with powder form.