▎ 摘　　要

Here we reported a simple method to tailor vertically graphene architecture in polydimethylsiloxane composite with high thermal conductivity. The few-layer graphene with lateral dimensions of around 500 nm and thickness of similar to 2 nm was exfoliated with hyperbranched polyethylene as stabilizer via CH-pi interactions against re-stacking. Vertically structure in composite was delivered by layer alternating graphene film, and the thermal conductivity is 2.18 W.m(-1).K-1, which is mainly due to the formation of effective heat transfer route through aligned nanosheets. This work demonstrates that polymer composite with vertically graphene architecture is a promising candidate for thermal interface materials.