Ultrahigh Thermal Conductive yet Superflexible Graphene Films

Electrical devices generate heat at work. The heat should be transferred away immediately by a thermal manager to keep proper functions, especially for high‐frequency apparatuses. Besides high thermal conductivity ( K ), the thermal manager material requires good foldability for the next generation flexible electronics. Unfortunately, metals have satisfactory ductility but inferior K (≤429 W m −1 K −1 ), and highly thermal‐conductive nonmetallic materials are generally brittle. Therefore, fabricating a foldable macroscopic material with a prominent K is still under challenge. This study solves the problem by folding atomic thin graphene into microfolds. The debris‐free giant graphene sheets endow graphene film (GF) with a high K of 1940 ± 113 W m −1 K −1 . Simultaneously, the microfolds render GF superflexible with a high fracture elongation up to 16%, enabling it more than 6000 cycles of ultimate folding. The large‐area multifunctional GFs can be easily integrated into high‐power flexible devices for highly efficient thermal management.