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Hollow carbon microspheres were successfully fabricated in a convenient fashion by employing polyacrylonitrile (PAN) emulsions as precursors. The obtained hollow carbon microspheres were shown high monodispersity, tunable pore structures-gradient pore diameters and uniform orientation of pores. Through varying the flowing rates of three phases and solidification time, the PAN microspheres with different sizes and densities could be simply synthesized. Besides the relationship between the solidification time and the density of microspheres as well as their gas barrier properties were studied in this paper. These structured microspheres have great potential applications in various areas, including foam targets, carbon molecular sieve, cargo storage, medical instruments and so on.