This work designed a series of three-way catalysts (TWCs) with and without the modification by La 0.67 Fe 0.83 Cu 0.17 O 3 (LaFeCu) perovskite to reduce the formation of N 2 O and NH 3 emissions from natural gas vehicles (NGVs). The modified PtRh catalyst was found to have an efficient TWC performance and to reduce the formation of N 2 O and NH 3 significantly. The Xray diffraction and CO-Fourier transform infrared results demonstrated the formation of Rhx species, which would reduce the formation of NCO*, the main precursor of NH 3 . In situ diffuse reflectance infrared Fourier transform spectroscopy was used to confirm that no NCO* groups were found on the modified catalyst. The X-ray photoelectron spectroscopy results revealed the increase in the Pt 2+ content on the modified catalyst, promoting the decomposition of N 2 O. Also note that the modified catalyst produced far fewer N 2 O than the catalyst without modification in the model reaction of CO + NO. Our work would provide a solution to develop an advanced TWC for NGVs.