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On page 677, M. Q. Zhao et al. report the fabrication of a hierarchical composite combining one-dimensional single/double walled carbon nanotubes (CNTs) and two-dimensional flakes through direct carbon deposition on layered double hydroxides. The composites can be easily transformed into continuously interlinked CNT layers alternating with calcined lamellar flakes structure. They are found to have the potential for applications in a number or areas, including as an excellent filler for strong polyimide film.