Two-dimensional network-structured carbon nanoscale building blocks, going beyond graphene, are of fundamental importance, and creating such structures and developing their applications have broad implications in environment, electronics and energy. Here, we report a facile route, based on electro-spraying/netting, to self-assemble two-dimensional carbon nanostructured networks on a large scale. Manipulation of the dynamic ejection, deformation and assembly of charged droplets by control of

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... or cone instability and micro-electric field, enables the creation of networks with characteristics combining nanoscale diameters of one-dimensional carbon nanotube and lateral infinity of two-dimensional graphene. The macro-sized (meter-level) carbon nanostructured networks show extraordinary nanostructural properties, remarkable flexibility (soft polymeric mechanics having hard inorganic matrix), nanoscale-level conductivity, and outstanding performances in distinctly different areas like filters, separators, absorbents, and wearable electrodes, supercapacitors and cells. This work should make possible the innovative design of high-performance, multi-functional carbon nanomaterials for various applications.