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In this study, a nitrogen–phosphorus intumescent flame-retardant 3-(N-diphenyl phosphate) amino propyl triethoxy silane (DPES), the ionic liquid (IL) of 1-butyl-3-methyl-imidazole phosphate, and a phosphorous-containing ionic liquid-modified expandable graphite (IL-EG), were synthesized, and their molecular structures were characterized. The flame-retardant rigid polyurethane foams (RPUFs) were compounded with synergistic flame-retardant IL-EG/DPES to study the effects of the combination IL-EG and DPES on the pore structure, mechanical properties, thermal decomposition behavior and thermal decomposition mechanism of RPUF. The results showed that IL-EG/DPES had good thermal stability, and an excellent expansibility and char yield. The flame-retardant RPUF, modified with IL-EG and DPES at the ratio of 1:1, had a relatively uniform pore size, the highest compressive strength, and an excellent flame-retardant performance due to the form interwoven hydrogen bonds between IL-EG and DPES, as well as the new synergistic flame-retardant coating on the RPUF surface to restrict the transfer of gas or heat into the PU matrix. [ABSTRACT FROM AUTHOR]