Membranes for membrane distillation (MD) are mostly made of polymeric and ceramic materials. We demonstrate here that the laterally-compressed, vertically-aligned CNTs (VACNT) obtainable from a CNT forest are an excellent membrane material for vacuum membrane distillation (VMD). The VACNT structure provides interstices between CNTs for extracting vaporized water molecules, while efficiently filtering the impurity salts. The VACNT membrane is shown to deliver excellent performance when tested for the desalination of 3.5 wt% NaCl water solution, as exemplified by the permeability of 68 LMH (liter per square meter per hour) achieved at the salt rejection of over 99.8% at 65 °C. We also demonstrate that the VACNT membrane performance can be maintained with time with the aid of a simple cleaning procedure, which bodes well for a long lifetime of the membrane for VMD application.