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Graphene (nano) platelets (GPs) are cost‐effective and possess high structural integrity, but their limited surface functional groups hinder their compatibility with polymers. In this study, an eco‐friendly, water‐based mechanochemical approach was developed to modify GPs with polyacrylamide (PAM), creating PAM graphene platelets (PAM‐GPs) with a grafting ratio of approximately 15%. The platelet was measured to be a few nanometers in thickness, and the grafted PAM provides abundant functional groups, including amide groups, which enhance compatibility with polymers. A typical polymer, bisphenol‐A epoxy, was compounded with PAM‐GPs, resulting in a high degree of exfoliation and dispersion of PAM‐GPs within the matrix. The resulting epoxy/PAM‐GP composites exhibited significantly improved mechanical properties, including an 18% increase in Young's modulus and a substantial enhancement in fracture toughness, with a 71% increase at a low filler fraction of 0.5 wt%. These improvements are attributed to the effective interfacial interaction between the PAM‐GPs and the epoxy matrix, facilitated by the grafted functional groups. This study highlights the potential of PAM‐GPs as toughening fillers for epoxy composites, emphasizing their applicability in enhancing the durability and performance of structural components in industrial applications. Highlights: Polyacrylamide (PAM)‐modified graphene platelets by a water‐based approach.A strong interface promoted exfoliation and dispersion of platelets.PAM‐modified platelets improved epoxy modulus and toughness.Fractographic analysis unveils toughening mechanisms. [ABSTRACT FROM AUTHOR]