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Flexible and highlyfifilled conductive polymer composites with strong mechanical properties are highlydesirable as electromagnetic interference (EMI) shielding and thermally conductive materials for humanprotection and wearable devices. Herein, a tough interface has been built up by the combination ofpolydopamine modifification and pH triggered hydrogen bonding to prepareflflexible and mechanicallyrobust waterborne polyacrylate/graphene@polydopamine composites. Graphene was modifified withpolydopamine via an in-situ polymerization method. By adjusting the initial pH value in thefifilm formation process, the transition from electrostatic repulsion to hydrogen bonding between graphene@polydopamine and polyacrylate was engineered for improving the mechanical properties. At optimalpH value, the maximum tensile strength of the composite is enhanced by 137% compared with that ofneat polymer matrix. Moreover, the composite withfifiller loading of 20 wt% exhibits an EMI shieldingeffectiveness of 58 dB at 0.6 mm thickness and thermal conductivity of 1.68 W/m$K, respectively. Thepractical application of the compositefifilm and composite coated leather also demonstrates theiroutstandingflflexibility, EMI shielding, and heat dissipation performance, indicating their excellent potential as EMI shielding and thermally conductive materials in wide areas such as wearable devices,telecommunication systems, and human protection.©2021 Elsevier Ltd. All rights reserved