A multiwall carbon nanotube/graphene (MWCNT/GR) composite was synthesized for an enhanced supercapacitor. Aerosol spray drying (ASD) was used to synthesize the MWCNT/GR particles using a mixture of graphene oxide (GO) solution and MWCNT. The effect of the ratio of the MWCNT/GO on the composite properties, including the shape and layered structure, was investigated. The MWCNT/GR composites with a morphology were generally a crumpled paper ball in shape, and the average diameter of MWCNT/GR particle was approximately 5 μm. MWCNTs were uniformly dispersed in graphene sheets and the MWCNTs not only increased the basal spacing but also bridged the widely spaced layers for better electron transfer between graphene sheets. Thus, the MWCNTs increased the contact area of electrolyte/electrode and facilitated ion transportation of electrons and electrolyte in the electrode. Electrochemical results demonstrate that the MWCNT/GR (weight ratio = 0.1) electrode has a capacitance of 192 F g-1 and excellent rate of capacity retention (88% at 4 A g-1), using a two-electrode testing system.