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Copper-aluminum layered double hydroxides (Cu-LDHs) and nickel-aluminum layered double hydroxides (Ni-LDHs) were synthesized using co-precipitation method. LDHs were organically modified by long chain sodium stearate. Polypropylene (PP)/layered double hydroxides (LDHs) and polypropylene (PP)/organically-modified layered double hydroxides (m.Cu-LDHs or m.Ni-LDHs) were prepared through the melt bending of the PP with either nanosized LDHs or m.LDHs without any other additives. The effect of stearate on the dispersibility of LDHs was investigated by X-ray diffraction (XRD). The surface morphology of LDHs was also studied using scanning electron microscope (SEM), and the thermal stability properties of PP/LDHs composites were studied by thermogravimetric analysis (TGA). The mechanical properties of the PP/LDH composites, tensile strength, and modulus of elasticity were investigated. The flammability properties were investigated using the cone calorimeter test. The intercalation of modified LDHs was determined by XRD in the presence of stearate. Results showed that modified LDHs presented good disperasbility in the PP matrix. The thermal stability of PP has been improved by up to 6% using m.Ni-LDHS. Unmodified and modified nanosized LDHs decreased the fire growth rate of PP from 10.8 kW/m2.s to 4.1 kW/m2.s and 4.5 kW/m2.s, respectively.