Reported powdery adsorbents with poor adsorption efficiency and stability make it imperative to develop novel materials to extract gallium ions (Ga(III)) from effluents. Herein, UiO-66-NH2-based mixed matrix membranes (TPU/0.1THB/U6N-1.5 MMMs) via electrospinning is firstly reported for separation and recovery of Ga(III). TPU/0.1THB/U6N-1.5 MMMs efficiently overcomes multiple bottlenecks of powder UiO-66-NH2, including poor stability, reusability and adsorption capacity. Its maximum adsorption for Ga(III) is 96.18 mg.g(-1) at pH 10.0. It has superiority in selective adsorption of Ga(III) from Al(III), Cu(II), Zn(II), Co(II) coexistence solution. Adsorption capacity of TPU/0.1THB/U6N-1.5 for Ga(III) reaches more than 80% after 9 cycles. Specially, it still retains excellent mechanical strength, flexibility and structural integrity after 12 h filtration, or after 9 adsorption-desorption cycles, even soaked in 5 mol.L (-1) HCl for a week. TPU/0.1THB/U6N-1.5 MMMs also improves the problem of low water flux. TPU/0.1THB/U6N-1.5 with high MOFs loading possess high water flux of 382.2 L.m(-2) .h(-1) with a permance of 382.2 L.m(-2).h(-1).bar(-1) and rejection rates of 90% for Ga(III). The main adsorption mechanism of TPU/0.1THB/U6N-1.5 is based on the chelation between phenolic hydroxyl groups of MMMs and Ga(III) at pH 10.0. Overall, the as-prepared TPU/0.1THB/U6N-1.5 has potential for water treatment through the process of membrane adsorption.