The novel nanocomposites derived from waterborne polyurethane (WPU)/Attapulgite (AT) nanocomposites have been successfully synthesized by in situ polymerization progress. AT functionalized by chemical modification were incorporated as a crosslinker in prepolymer. The chemical structures, morphology, thermal behavior, and mechanical properties of the WPU/AT nanocomposites were investigated by Fourier transform infrared spectroscopy (FTIR), thermo gravimetric analysis (TGA), differential scanning calorimetry (DSC), scanning electron microscopy (SEM), X-ray diffraction (XRD) and tensile testing respectively. The experimental results indicated that the organically modified attapulgites were homogeneously dispersed in the WPU and resulted in an improvement of thermal stability, tensile strength and elongation at break of WPU/AT nanocomposites.