Desalination by membrane distillation (MD) using low-grade or waste heat provides a potential route for sustainable water supply. Nonwetting, porous membranes that provide a selective pathway for water vapor over nonvolatile salt are at the core of MD desalination. Conventional water-repelling MD membranes (i.e., hydrophobic and superhydrophobic membranes) fail to ensure long-term desalination performance due to pore wetting and surface fouling. To address these challenges, a defect-free carbon nanotube forest (CNTF) is engineered in situ on a porous electrospun silica fiber substrate. The engineered CNTF forms an ultrarough and porous interface structure, allowing outstanding wetting resistance against water in air and oil underwater. As a result of this antiwetting property, the composite CNTF membrane displays a stable water vapor flux and a near complete salt rejection (>99.9%) in the desalination of highly saline water containing low surface tension contaminants. The antimicrobial property of the composite CNTF membrane imparted by the unique forest-like architecture and the oxidative effect of carbon nanotubes (CNTs) are further demonstrated. The results exemplify an effective strategy for engineering CNT architecture to elucidate the structure-property-performance relationship of the nanocomposite membranes and to guide the design of robust thermal desalination membranes. and the inability of RO to desalinate high-salinity waters are major practical challenges. [2] Membrane distillation (MD) is an emerging thermal-driven desalination technology, capable of using low-grade or waste heat to drive selective permeation of water vapor over nonvolatile species (e.g., salt) through a porous hydrophobic membrane. [3] MD is highly advantageous for desalinating hypersaline brines that cannot be treated by RO desalination. However, MD desalination performance is significantly hampered by the inability of conventional hydrophobic membranes to maintain long-term antiwetting and antifouling properties, particularly in the presence of low surface tension contaminants in the feed water. [4] Thus, developing high-performance MD membranes with robust wetting and fouling resistance is crucial for widespread adoption of MD desalination.Recent studies have demonstrated the fabrication of MD membranes with improved wetting resistance by tailoring the surface chemistry and nanostructure. [5] Specifically, the membrane surface in these studies was functionalized with extremely low interfacial energy materials, such as fluoroalkylsilane (FAS), to reduce the surface free energy and thus the attraction of water molecules. Ultralow interfacial energy modification results in a surface exhibiting a water contact angle >90°, regardless of surface morphology. [6] To have an oil-repelling nature as wellan important property for treatment of waters containing oil and Carbon Nanotube Forests