A graphene and carbon nanotube (CNT) array composite was synthesized by chemical vapor deposition (CVD) and chemically treated after synthesis, yielding a novel corrugated structure, visually similar to a mushroom gill. This binder-free hybrid material was used to make an electrode that may find application in energy storage devices, such as supercapacitors. The electrode performance of the corrugated graphene/CNT array composite (CGCC) was compared to that of commercial glassy carbon. The results of the comparison are presented here, along with suggestions for further development of the CGCC electrode.