Graphene oxide (GO) and reduced graphene oxide (RGO) platelets were pillared with carbon nanotubes (CNTs) by using the chemical vapor deposition (CVD) method with acetonitrile as the carbon source and nickel nanoparticles as the catalyst, aimed to prepare graphene-based materials with a high surface area and a good electrical conductivity. Characterization data showed that the composite materials with RGO layers pillared by CNTs formed a robust three-dimensional (3D) porous structure of specific surfaces as high as 352 m2/g. The amount and length of the CNT pillars connecting the RGO layers were controlled by changing the amount of the nickel metal catalyst and the time of CVD. The CNT-pillared RGO composite materials exhibited an excellent visible light photocatalytic performance in degrading dye Rhodamine B because of the unique porous structure and the exceptional electron transfer property of graphene. Such CNT−RGO composites represent a new family of innovative carbon materials for visible-light-activated photocatalysis.