A novel halogen-free flame retardant (FR) consisting of brucite, aluminum phosphate (AlP), and silane coupling agent (B/AlP/A) was prepared via co-precipitation assembly technique. The morphology, chemical compositions, size distribution, and thermal stability of B/AlP/A were investigated. When used in ethylene-vinyl acetate (EVA) resin, the B/AlP/A could significantly enhance the flame retardant and smoke suppression performance of the EVA composites, which is mainly attributed to the AIP. With 50 wt% FR loading, the peak heat release rate (PHRR) of EVA-B/AlP/A (299.2 kW Á m −2) is much lower than that of EVA-B/A (387.4 kW Á m −2). Moreover, B/AlP/A shows an excellent smoke suppression performance. For example, the smoke production rate is 0.017 m 2 Á g −1 that has been decreased by 72.1%, compared with B/A. The improvement arises from the amorphous AlP layer on brucite, which helps to create a firm and porous protective char layers on the burning EVA composites. Meanwhile, better mechanical property could be simultaneously obtained with the large FR amount. The fluffy surface of B/AlP/A has good compatibility with EVA and tangle more polymer chains, enhancing the mechanical properties. In a word, this simple and convenient method could pave the way for developing a more efficient and cost-effective brucite-based FR.