Developing efficient methods to prepare high-performance flame retardant and smoke suppression wood is crucial for the application. Herein, nanostructured poplar wood (DWI-4) with remarkable flame retardant and smoke suppression performance was fabricated by impregnating ammonium dihydrogen phosphate (ADP) and nano-silica (SiO2) into delignified wood (DW-4). With the delignification treatment, lignin was partially removed, and numerous pores and cracks were developed on the cell wall of wood, allowing more ADP-SiO2 particles to be impregnated into wood. As a result, ADP-SiO2 particle was not only anchored in the lumens (pores) of wood, but also was penetrated and embedded into the cell wall, achieving the synergistic modification of the lumen and cell wall of wood. As anticipated, the produced DWI-4 featured outstanding flame retardant and smoke suppression performance. The peak heat release rate (pHRR) of DWI-4 was as low as 38.2 kW m−2, which was only 8 % of that of natural wood (NW). And the total heat release (THR) and total smoke production (TSP) demonstrated reductions of 73.9 % and 64.4 % comparing to NW. Moreover, the compressive strength of DWI-4 increased by 31.4 % comparing to NW. The structure of residual char of DWI-4 was more stable and the gas intensity produced by the combustion of DWI-4 decreased remarkably. Therefore, the synergy of delignification and ADP-SiO2 impregnation significantly enhanced the flame retardant and smoke suppression performance of wood and the enhanced mechanism was revealed. The nanostructured poplar wood with excellent flame retardant and smoke suppression performance was prepared, providing an effective method for the functional improvement of wood and expanding the fields of application.