The development of lightweight and integration for electronics requires flexible films with high thermal con-ductivity and electromagnetic interference (EMI) shielding to overcome heat accumulation and electromagnetic radiation pollution.Herein,the hierarchi-cal design and assembly strat-egy was adopted to fabricate hierarchically multifunctionalpolyimide composite films,with graphene oxide/expanded graphite (GO/EG) as the top thermally conductive and EMI shielding layer,Fe3O4/polyimide (Fe3O4/PI) as the middle EMI shielding enhancement layer and electrospun PI fibers as the substrate layer for mechani-cal improvement.PI composite films with 61.0 wt% of GO/EG and 23.8 wt% of Fe3O4/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.