The organically-modified layered zinc phenylphosphonate (m-PPZn) were prepared by a facile chemical intercalation method. Poly(1,4-butylene adipate) (PBA) belonged to biodegradable polymers and was friendly to environment. Thus, the solution-casting method was used to obtain the new PBA/m-PPZn nanocomposites. Crystallization kinetics and morphology of PBA and 0.5wt% PBA/m-PPZn nanocomposites were studied using differential scanning calorimetry (DSC), polarizing optical microscopy (POM), transmission electron microscopy (TEM), and wide-angle X-ray diffraction (WAXD). Both WAXD and TEM results illustrated that most of the layered materials of partial delamination are randomly dispersed in the PBA matrix. The crystallization time increased with increase in crystallization temperature for neat PBA and 0.5wt% PBA/m-PPZn nanocomposites. When compared to neat PBA, the t1/2 of the fabricated 0.5 wt% PBA/m-PPZn nanocomposites demonstrated significant decreased under the same isothermal crystallization conditions. This indicates that the incorporation of the m-PPZn content into PBA significantly enhances the crystallization rate of PBA. With the presence of m-PPZn, the nuclei number of PBA increases and the spherulite size significantly reduces. Therefore, the addition of m-PPZn to PBA induces heterogeneous nucleation.