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Enhancing the flame retardancy with minimal impact on the mechanical and thermal performances of polymers remains a challenge. This study synthesized a phosphorus/nitrogen‐containing silane compound (D) using polyformaldehyde, KH‐550, and 9,10‐dihydro‐9‐oxa‐10‐phosphaphenanthrene‐10‐oxide (DOPO) as raw materials through the Kabachnik‐Fields reaction. After that, D was grafted onto the surface of graphene after hydrothermal treatment to obtain a nano hybrid flame retardant (D‐GR). And D‐GR/EP composites exhibited good flame resistance (LOI = 30.1% and UL‐94 reaches the V‐1 rating) even if the load on D‐GR was 1 wt%. Indeed, the total heat release, the peak heat release rate (PHRR), and the total smoke release of 1% D‐GR/EP dropped by 13.54%, 28.62%, and 44.32%, respectively, in comparison to pure EP. The mechanical performance of 1% D‐GR/EP was effectively maintained, as indicated by the results of impact, tensile and flexural tests. A systematic evaluation indicated that the accession of D‐GR effectively inhibited smoke and heat releases that are ascribed to the synergistic effect of phosphorus/nitrogen‐containing silane compound and graphene. In this study, a facile method was provided for the synthesis of halogen‐free flame‐retardant epoxy composites with superior performances. The combustion products of the as‐prepared composites complied with green and environmental protection standards.