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The development of lightweight and integration for electronics requires flexible films with high thermal conductivity and electromagnetic interference (EMI) shielding to overcome heat accumulation and electromagnetic radiation pollution. Herein, the hierarchical design and assembly strategy was adopted to fabricate hierarchically multifunctional polyimide composite films, with graphene oxide/expanded graphite (GO/EG) as the top thermally conductive and EMI shielding layer, Fe 3 O 4 /polyimide (Fe 3 O 4 /PI) as the middle EMI shielding enhancement layer and electrospun PI fibers as the substrate layer for mechanical improvement. PI composite films with 61.0 wt% of GO/EG and 23.8 wt% of Fe 3 O 4 /PI exhibits high in-plane thermal conductivity coefficient (95.40 W (m K) −1 ), excellent EMI shielding effectiveness (34.0 dB), good tensile strength (93.6 MPa) and fast electric-heating response (5 s). The test in the central processing unit verifies PI composite films present broad application prospects in electronics fields.

Hierarchically Multifunctional Polyimide Composite Films with Strongly Enhanced Thermal Conductivity