In this manuscript, flame-retardant and smoke-suppressant flexible polyurethane foams (FPUFs) were designed and synthesized based on novel liquid phosphorus-containing polyol named as PDEO and expandable graphite (EG). The reactive PDEO can be chemically added into the chain of FPUF, while expandable graphite was blended into the matrix of foam through foaming process. Benefitting from the incorporation of reactive PDEO with a long chain, the resultant FPUF containing EG exhibited considerable mechanical properties. More importantly, the synergistic effect of PDEO and EG can endow FPUF with great flame retardancy, anti-driping performances. Furthermore, the resultant FPUF/EG/PDEO foams exhibit considerable smoke suppression performances. The vertical burning test revealed that the FPUF containing 5 php PDEO and 10 php EG extinguished quickly without dripping and kept the original shape after removing the igniter. The cone calorimeter results demonstrated that the synergistic effect of PDEO and EG can effectively reduce the heat release rate (HRR) and total release rate (THR) of the composite foam. Remarkably, the smoke production release (SPR), total smoke production (TSP), light transmission and specific optical density results indicated significantly smoke-suppressant properties of the composite foam. The mechanism analysis confirmed that the synergistic effect of gas condensed bi-phase action from PDEO and EG contributed the great flame retardation of the composite foam. This novel FPUF provides a promising strategy for producing the polymer foam with flame retardation, smoke suppression and anti-dripping performances.