Flexible polyurethane foam (PUF) is coated by layer-by-layer (LbL) assembly using branched polyethyleneimine (BPEI), poly (acrylic acid) (PAA), and two different charged nanoparticles, such as sodium montmorillonite (Na-MMT) and layered double hydroxide (LDH). Three different deposition strategies, that is, bilayer, trilayer, and quadlayer, exhibit different coating growth, morphology, and flammability properties. Changing the nanosheet from LDH to Na-MMT dramatically alter the coating mass for the same number of layers. A five bilayer PAA/BPEI1LDH coating reduced the peak heat release rate by 40% and the average heat release rate by 70%, which is two times more effective than commercial fire retardants (FRs) and other LbL-FR coatings for PUF. Na-MMT and LDH mixed multilayers resulted in effective flame-retardant coatings with less coating mass by manipulating the deposition strategy. This study manifests the flexibility of LbL to fine-tune flammability reduction by switching the coating weight gains, which is significant to accelerate the development of other LbL coating regardless of the intended applications.