Layer-stacking structures via the template-free synthesis are rare in two-dimensional microporous organic networks (2D MONs). Herein, we report a facile solvent regulation and template-free strategy by tuning the aggregation degree of 2D β-cyclodextrin (CD)-based MONs nanosheets. The 2D MON nanosheets provided larger uptake capacity and faster kinetics than the aggregated CD-MONs, revealing the significance of morphology control for the removal of pollutants. The prepared 2D CD-MON-DMF gave ultrafast adsorption kinetics and exhibited much larger saturation sorption capacity (327.9 mg g⁻¹) than previous adsorbents for bisphenol AF. The developed strategy not only provides a novel way to construct 2D MON nanosheets for highly efficient removal of organic pollutants from water but also promotes the utilization of MONs in material and environmental sciences.

通过无模板合成的层堆叠结构在二维微孔有机网络（2D MONs）中很少见。在此，我们通过调整二维 β-环糊精 (CD) 基 MONs 纳米片的聚集度，报告了一种简便的溶剂调节和无模板策略。与聚集的 CD-MON 相比，2D MON 纳米片提供了更大的吸收能力和更快的动力学，揭示了形态控制对于去除污染物的重要性。制备的 2D CD-MON-DMF 具有超快的吸附动力学，并表现出更大的饱和吸附容量（327.9 mg g ^-1) 比以前的双酚 AF 吸附剂。所开发的策略不仅提供了一种构建二维 MON 纳米片以高效去除水中有机污染物的新方法，而且还促进了 MON 在材料和环境科学中的应用。