The reflectance spectrum of fresh plant leaves in the near infrared has been systematically analyzed. It is verified that presence of O-H is the key to those vegetation′s spectral characteristics at about 1450 nm and 1940 nm. Based on the knowledge, Mg-Al-X-LDH (X represents NO3-, Cl-, CO32-, SO42-), four types of novel spectral simulation materials containing interlayed O-H, were designed and prepared, and their X-ray diffraction patterns, infrared spectra, thermogravimetric curves and Raman spectra were characterized. The model calculation results of spectral correlation mapper and spectral angle mapper show similarities more than 0.9600 and 0.9700 between four types of layered double hydroxides (LDHs) and plant leaves in near infrared reflectance spectrum. The polyurethane coating with Mg-Al-Cl-LDHs as a simulation material exhibits a highly coincided spectrum with that of plant leaves, and similarities of two calculation models are up to 0.9702 and 0.9924, respectively. The similarities calculation of reflectance spectra for Mg-Al-Cl-LDHs before and after calcining at 180 ℃ are still up to 0.9888 and 0.9959, indicating high thermo stability of Mg-Al-LDHs.