In this study, the organically-modified layered zinc phenylphosphonate (m-PPZn) prepared using coprecipitation method were sucessfully synthesized to intercalate hexadecylamine into the interlayer spacing of PPZn. The interlayer spacing of m-PPZn determined by wide-angle X-ray diffraction (WAXD) was increased from 14.5 Å for PPZn to 27.9 Å for m-PPZn. These results suggest that the hexadecylamine were successfully exchanged and intercalated into the interlayer spacing of PPZn. The poly(butylene succinate/adipate)(PBSA)/m-PPZn nanocomposites were then prepared by melt-mixing. The structure, morphology, and crystallization behavior of the PBSA/m-PPZn nanocomposites were characterized using WAXD, transmission electron microscopy (TEM), and differential scanning calorimetry (DSC). Both WAXD and TEM results demonstrate that most of the partial-delamination m-PPZn was randomly dispersed in the PBSA matrix. With the addition of 5wt% m-PPZn, the crystallization temperature (Tc) of the PBSA/m-PPZn nanocomposites was increased about 3.84 oC compared with that of neat PBSA using non-isothermal crystallization method. It has been shown that m-PPZn containes an effective nucleating effect for PBSA.