This research is to elucidate the impact of carbon nanomaterials in electrospun membranes that are applied in membrane distillation. Different carbon nanomaterials including carbon black, carbon nanotubes and graphene oxide were incorporated into the polymer-based electrospun membranes. The membrane distillation performance was investigated by employing the fabricated membranes in a self-made setup. The physical properties of membranes were characterized and related to the membrane distillation performance by a self-developed theoretical model to understand the effect in various aspects. The experimental results revealed the impacts of membrane morphology, hydrophobicity and pore formation. And the simulation results indicated that the current proposed mechanisms are not sufficient to explain the performance of nanocomposite membranes. More promising endeavor was presented to further understand the mechanism.