ABSTRACT:The “brick-like” N-doped graphene-carbon nanotube (NGC) composites are designed by mechanically grinding the filtration films, which are fabricated to form a three-dimensional structure film as a counter electrode (CE). The N-doped graphene/carbon nanotube films with a three-dimensional “brick-like” structure can provide numerous vertical active edge sites. The excellent electrochemical catalytic ac-tivities of CE can be obtained by adjusting the different ratio of graphene to CNTs to control the size and N-doping content of breaking particles. NGC17 CE based dye-sensitized solar cells (DSSC) have reached a high efficiency (6.74%) close to platinum-based cells (6.89%). The excellent efficiency may be attributed to the following factors: a) the DEP of NGC17 (304 mV) is lower than that of the Pt electrode (389 mV); b) the charge transfer resistance (Rct) at the NGC17-CE/electrolyte interface was 1.78 U cm-2, which is lower than that of a Pt-CE/electrolyte interface (8.97 U cm-2).