Membranes with ultrathin rejection layers can effectively achieve high water permeability. In the current study, we report a single-step fabrication of carbon nanotubes (CNTs)-loaded ultrathin film composite (uTFC) polyamide membranes using an electrospray-assisted interfacial polymerization method. In this method, amine and acyl chloride monomer solutions were electrosprayed into micro-droplets to allow a controlled growth of the polyamide rejection layer. At the same time, CNTs were uniformly dispersed under the action of the electrical field. The loading of CNTs in the polyamide rejection layer markedly enhance the water permeability of the membrane with a 2-6 folds enhancement. The simple and versatile electrospray-assisted interfacial polymerization method, which allows simultaneous control of rejection layer thickness and dispersion of nanomaterials, paves a new dimension for the preparation of high performance ultrathin nanocomposite membranes.