Emerging Janus membranes, named after the ancient Roman god with two faces to better survey both the past and the future, are appealing materials to tackle this challenge. They possess opposing chemicophysical properties on two sides for achieving a breakthrough in their performances. [12] The opposite surface properties usually include asymmetric wettability and charge but not limited to them. [13] Janus membranes with asymmetric wettable surfaces have received most of the attention in diverse research fields for a wide variety of applications because of their distinctive mass (e.g., liquid or gas) transport behaviors in two-phase or multiphase systems. Such unique fluid transportation relies on the cooperative effect arisen from the asymmetric wettability in the direction of membrane thickness. [14] Therefore, how to create and regulate asymmetry is a core task in the preparation of Janus membranes.Surface engineering, a process for modifying the surface of a material, provides a powerful toolbox to enhance and optimize the performance of the material, especially for porous membranes with large internal surface area. A myriad of modification methods including surface coating, grafting, and self-assembling have been developed to regulate membrane surface properties which are usually uniform in the spatial distribution. As distinguished from ordinary surface treatments, asymmetric surface engineering aims to accurately control the uneven distribution of surface properties or functionalities in the direction of membrane thickness, being an effective means for the preparation of Janus membranes.Benefiting from the asymmetric surface engineering, the researches on Janus membranes have mushroomed in recent years. Hundreds of literatures have explored the possibilities for Janus membranes to substitute traditional ones for achieving enhanced performances in the mass transfer between two phases, including water−oil, water−gas, and oil−gas systems. Some researchers have reviewed the research progresses on Janus membranes from different perspectives. Our previous review has discussed the definition and fabrication of Janus membranes and summarized their applications in the field of environmental science. [13] Another two reviews, presented by Zhao et al. [14] and Zhou et al., [15] have described the distinctive unidirectional fluid transport phenomenon of Janus membranes and their functional applications. Besides, a recent review has detailed the potential of Janus configuration in terms of enhancing energy efficiency in membrane processes. [12] However, the vital role of asymmetric surface engineering in the construction of asymmetric configurations, the modulation of surface properties, and the implementation of ultimate applications has not been addressed. Herein, Janus membranes show great promise toward various applications and are undergoing a fast-paced development in materials science. The asymmetric surface engineering on surface wettability, layer thickness, and pore structure enables Janus membranes with super...