Since the commercialization of rechargeable lithium-ion batteries (LIBs) in 1991, they have become the ubiquitous power sources for portable electronic devices, electric vehicles, and grid electricity storage. Over the past three decades, extensive research efforts have been invested to develop new generations of cathode and anode materials with enhanced cycling performance. Nonetheless, graphite is still the dominant anode for commercial LIBs because of its superior reversibility of Li de-/intercalation and low cost. Graphite is a layered material consisting of graphene sheets, which have strong covalently bonded carbon atoms forming a network of honeycombs in each layer. The binding forces between each layer arise from weak dispersion or van der Waals (vdW) interactions, enabling the intercalation of ionic and molecular species. Upon Li intercalation, the vdW interactions are screened, and the graphene layers glide with respect to each other, resulting in a symmetry change from an AB stacking (see Figure ) in graphite (C 6 ) to an AA stacking (see Figure Schrodinger Inc., New York, NY 10036. E-mail: jianli.cheng@schrodinger.com † Electronic Supplementary Information (ESI) available.