▎ 摘　　要

Innovations of transistors toward miniaturization and integration aggravate heat accumulation of central processing units (CPUs). Thermal interface materials (TIMs) are critical to remove the generated heat and to guarantee the device reliability. Herein, maltose-assisted mechanochemical exfoliation was proposed to prepare maltose-g-graphene as a structural motif of TIMs. Then, maltose-g-graphene/gelatin composite films with a bilayer structure were prepared by two-step vacuum filtration to construct effective thermally conductive pathways consisting of the directionally arranged and tightly packed maltose-g-graphene. The bilayer composite film exhibited a remarkable in-plane thermal conductivity (30.8 W m(-1) K-1) and strong anisotropic ratio (similar to 8325%) at 40 wt % maltose-g-graphene addition. More intriguingly, the cooling effect on CPUs was significantly better for the bilayer composite films than commercial thermal pads as TIMs. The outstanding thermally conductive stability in resistance to instantaneous and prolonged thermal shocks as well as fatigue stability was gathered. Our work offers a valuable reference to design and fabricate high-performance TIMs for CPU cooling to surmount harsh application scenarios.