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It is a great challenge to improve the flame retardancy of polymer materials by adding eco-friendly magnesium hydroxide (Mg(OH)2) but simultaneously maintain satisfied mechanical performances. In this study, expanded graphite (EG) as a synergist was introduced into poly(butylene succinate) (PBS)/Mg(OH)2 system to investigate the effect of EG on their flame retardancy, thermal stability and mechanical properties. The results showed that only addition of 5 wt% EG into PBS/20 wt%Mg(OH)2 resulted in excellent flame retardancy, including that the LOI was 29.4%, the UL-94 rating reached to V0, and the PHRR decreased by 73%. These flame retarded parameters were comparable or even better than that of PBS/40 wt%Mg(OH)2 composites. More importantly, PBS/20 Mg(OH)2/5 EG presented much better thermal stability and mechanical properties than PBS/40 wt%Mg(OH)2, indicating a balanced improvement on comprehensive performances of PBS. Based on the comparison with PBS/20 Mg(OH)2/5Graphene(Gr) system and the structure analysis for residual chars, the mechanism for improved flame retardancy was attributed to the formation of gradient-structured char layer due to the helpful thermal expansion process of EG together with the decomposition of Mg(OH)2 during combustion, resulting in better barrier action to heat, oxygen and flammable gases via “labyrinth effect”. As far as we know, it is the first report that gradient-structured char layer was discussed in flame retarded polymer systems. Hence, this work provides not only a high-efficient synergist to improve the flame retardant efficiency of Mg(OH)2, but also useful guidelines to design polymer composites with balanced comprehensive performances.