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Carbon materials, such as multi-walled carbon nanotube (MWCNT), single-walled carbon nanotubes (SWCNT), and graphene sheets (GNS), filling into polymer substrates can effectively improve performance of composite materials [1], [2]. The data presented here in this article illustrates the different impacts of GNS and MWCNT on the mechanical properties of polypyrrole (PPy)-based composites systems. PPy/GNS and PPy/MWCNT binary composites were added into poly(3,4-ethylenedioxythiophene) poly (styrene sulfonate) (PEDOT PSS) matrix. Changing