There is an increasing demand worldwide on advanced two-dimensional (2D) nanofibrous networks with applications ranging from environmental protection and electrical devices to bioengineering. Design of such nanoarchitectured materials has been considered a long-standing challenge. Herein, we report a direct electronetting technology for the fabrication of self-assembled 2D nanoarchitectured networks (nano-nets) from various materials. Tailoring of the precursor solution and of the microelectric field allows charged droplets, which are ejected from a Taylor cone, to levitate, deform and phase separate before they self-assemble a 2D nanofibre network architecture. The fabricated nano-nets show mechanical robustness and benefit from nanostructural properties such as enhanced surface wettability, high transparency, separation and improved air filtration properties. Calcination of the nano-nets results in the formation of carbon nano-nets with electric conductivity and titanium dioxide nano-nets with bioprotective properties.