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p-pstacking interface design strategy is proposed to prepare ultrathin andflflexible water-borne polymer/sulfonated graphene nanosheets (S-GNS) composite by a facile self-assembly method in latex. The waterdispersible S-GNS was made by modifying the GNS with aryl diazonium salt. Styrene was introduced intowater-borne polymer to formp-pstacking interaction with S-GNS. The composite shows good mechanical properties and high electromagnetic interference (EMI) shielding effectiveness (SE) in the Xband (8.2e12.4 GHz). By Raman spectra, tensile tests, and simulation calculation,p-pstacking interaction is proved to be an effective interface bonding to enhance the mechanical properties. With afifillerloading of 20 wt%, the tensile strength of composites is enhanced by 578%. The incorporation of 25 wt% SGNS leads to a high EMI SE of 21.5 dB at 0.05 mm thickness, which remains unchanged after 1000 timesbending. The specifific SE/thickness (SSE/t) of the composite is as high as 2663 dB cm2/g, outperformingthe ever reported materials with similarfifiller loading (25 wt%). The composite can be used as coating onthe surfaces of solids, indicating the great potential for wide application.©2019 Elsevier Ltd. All rights reserved.