This study aims to eliminate or suppress explosion accidents in powder preparation and storage systems of coal dust. The modified fly ash cenosphere (FAC) was used as an inner spherical shell carrier with carbamide impregnated. Carbamide/FAC composite suppressant with bilayer spherical shell was prepared by vacuum freeze-drying. The flame propagation and explosion performances of coal were tested, respectively. The results showed that the surface-loaded carbamide particles had a particle size of similar to 4 nm. With the increasing content of carbamide/FAC composite suppressant, the maximum flame length gradually decreased, and the explosion suppression effect was gradually improved. Nearly complete explosion suppression of coal could be achieved with an added amount of 40 wt% carbamide/FAC composite suppressant. The carbamide loaded in carbamide/FAC composite suppressant mainly acted in the 0-tau(1) stage to weaken (dP/dt)(max). FAC mainly but not solely acted on the stage of tau(1)-tau(2) to decrease P-max. Carbamide particles were highly efficient and responsive. The suppression mechanism of carbamide/FAC composite suppressant was proposed, which was micro-nano multiscale complementary effect and deceleration-depressurization coupling effect.