Owing to the lack of precise atomic-level control offered by existing fabrication techniques over the edge structures in bilayer graphene, experimental studies on the edge effects in bilayer graphene structures have so far largely remained unexplored. In this study, two fully cove-edged bilayer nanographenes (CBGs) are synthesized via organic synthesis approach. One of the prepared CBGs contains a cavity defect. The bilayer stacked structures of CBGs are unambiguously characterized.