Yuan-Hang Jin, Menghao Li, Xin Wang, Zhuo-Qin Wang, Xin Li, Ao Liu, Yongkang Zhu, Yafei Hu, Ying‐Wei Yang
Common membrane material preparation methods for oil–water separation face critical challenges, including complex structures, cumbersome procedures, and high energy consumption, which limit their large-scale applications. To tackle these problems, here we present a macrocycle construction strategy for superwettable polymer membranes using pillararenes. Specifically, a hydrazone-linked pillararene-based polymer (NP5-TOB) was synthesized through a facile room-temperature interfacial polymerization and subsequently assembled into robust membranes using vacuum-assisted filtration, enabling the synergistic regulation of wettability and surface roughness. NP5-TOB membrane efficiently separates various complex oil/water systems under prewetting conditions, achieving a separation efficiency exceeding 99% and a flux of up to 4858.35 L m –2 h –1, thus offering a promising route for the development of high-performance membranes with excellent separation potential.