Graphene
has been the subject of much research, with structural
engineering frequently used to harness its various properties. In
particular, the concepts of graphene origami and kirigami have inspired
the design of quasi-three-dimensional graphene structures, which possess
intriguing mechanical, electronic, and optical properties. However,
accurate controlling the folding process remains a big challenge.
Here, we report the discovery of spontaneous folding growth of graphene
on the h-BN substrate via adopting a simple chemical vapor deposition
method. Folded edges are formed when two stacked graphene layers share
a joint edge at a growth temperature up to 1300 °C. Using first-principles
density functional theory calculations, the bilayer graphene with
folded edges is demonstrated to be more stable than that with open
edges. Utilizing this novel growth mode, hexagram bilayer graphene
containing entirely sealed edges is eventually realized. Our findings
provide a route for designing graphene devices with a new folding
dimension.