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Carbon nanotubes (CNTs) represent a typical nanomaterial with many potential applications.With controlled assembly, CNTs can be arranged into various three-dimensional macroscopic structures with unexpected properties;extensively studied structures include vertically aligned arrays (forest), isotropic CNT sponges and sponge-array tandem composites.We have synthesized a gradient structures CNT bulk material with an orientation gradual transform from aligned array to nearly random isotropic sponges.