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p-p stacking interface design strategy is proposed to prepare ultrathin and flflexible 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 into water-borne polymer to form p-p stacking interaction with S-GNS. The composite shows good mechanical properties and high electromagnetic interference (EMI) shielding effectiveness (SE) in the X band (8.2e12.4 GHz). By Raman spectra, tensile tests, and simulation calculation, p-p stacking interaction is proved to be an effective interface bonding to enhance the mechanical properties. With a fifiller loading 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 times bending. The specifific SE/thickness (SSE/t) of the composite is as high as 2663 dB cm2 /g, outperforming the ever reported materials with similar fifiller loading (25 wt%). The composite can be used as coating on the surfaces of solids, indicating the great potential for wide application. © 2019 Elsevier Ltd. All rights reserved.