Therefore, the development of an efficient, low-cost, and low-energy purification technology is highly desirable for the efficient removal of micropollutants and VOCs from water.Of particular importance are organic micropollutants from polymers, pesticides, and pharmaceuticals such as bisphenol A (BPA), bisphenol S (BPS), and 2-naphthol (2-NO), which have become global health concerns. [3][4][5][6] Additionally, water-soluble VOCs, such as phenol, which often contaminate water sources, can be detrimental to ecological systems, even at low concentrations. [7] Adsorption is a common method for water remediation through the use of various adsorbents such as surfactant-modified zeolite, [8] molecularly imprinted polymers, [9] macrocycle-based polymers, [10][11][12] hybrid mesoporous silicas, [13,14] covalent organic frameworks, [15] and metal-organic frameworks. [16][17][18] Carbonaceous materials are also common adsorbent materials for water remediation, but they have slow uptake rates for micropollutants (on the order of hours). [19][20][21] However, after adsorption, used activated carbon requires high thermal energy to regenerate it. [22] Therefore, it is imperative to develop new adsorbent materials that can be economically synthesized from cheap precursors through simple synthetic procedures. Moreover, these adsorbent materials should be able to adsorb micropollutants with very high adsorption kinetics and should exhibit excellent recyclability and outstanding adsorption capacity.Recently, Dichtel et al. successfully demonstrated a series of macrocycle-based polymers that could rapidly remove organic micropollutants from water. [3] Seminal works have triggered researchers to tackle a multitude of organic porous polymers to improve the rapid and high adsorption capabilities of various micropollutants. However, the economic synthesis of robust porous adsorbents with high efficiency is still awaited, and watersoluble VOCs are difficult to remove using common adsorption methods. [23] General mechanisms for VOCs removal such as catalytic reaction [24][25][26][27][28] are most well-known, but recently, VOCsFreshwater shortage is becoming one of the most critical global challenges owing to severe water pollution caused by micropollutants and volatile organic compounds (VOCs). However, current purification technology shows slow adsorption of micropollutants and requires an energy-intensive process for VOCs removal from water. In this study, a highly efficient molecularly engineered covalent triazine framework (CTF) for rapid adsorption of micropollutants and VOC-intercepting performance using solar distillation is reported. Supramolecular design and mild oxidation of CTFs (CTF-OXs) enable hydrophilic internal channels and improve molecular sieving of micropollutants. CTF-OX shows rapid removal efficiency of micropollutants (>99.9% in 10 s) and can be regenerated several times without performance loss. Uptake rates of selected micropollutants are high, with initial pollutant uptake rates of 21.9 g mg −1 min −1 , which a...