Conversion of atmospheric water to sustainable and clean freshwater resources through MOF-based adsorbent has great potential for the renewable environmental industry. However, its daily water production is hampered by susceptibility to agglomeration, slow water evaporation efficiency, and limited water-harvesting capacity. Herein, a solar-assisted bimetallic MOF (BMOF)-derived fiber component that surmounts these limitations and exhibits both optimized water-collect capacity and short adsorption-desorption period is proposed. The proposed strategy involves utilizing bottom-up interface-induced assembly between carboxylated multi-walled carbon nanotube and hygroscopic BMOF on a multi-ply glass fiber support. The designed BMOF (MIL-100(Fe,Al)-3) skeleton constructed using bimetallic-node defect engineering exhibits a high specific surface area (1,535.28 m2/g) and pore volume (0.76 cm3/g), thereby surpassing the parent MOFs and other reported MOFs in capturing moisture. Benefiting from the hierarchical structure of fiber rods and the solar-driven self-heating interface of photothermal layer, the customized BMOF crystals realize efficient loading and optimized water adsorption-desorption kinetics. As a result, the resultant fiber components achieve six adsorption-desorption cycles per day and an impressive water collection of 1.45 g/g/day under medium-high humidity outdoor conditions. Therefore, this work will provide new ideas for optimizing the daily yield of atmospheric water harvesting techniques.