Based on the possibility to provide scientific clues for the inversion of diamond formation environment and the design of the diamond synthesis process, the paper studied the relationship between the surface morphology, the content of impurity nitrogen and hydrogen and the degree of order in structure of natural placer diamonds from the western Yangtze Craton by using the optical microscope, infrared spectroscopy and Raman spectroscopy. The results show that the surface morphology on diamond includes micro-morphology related to crystal growth, ablation morphology depend on crystal orientation, ablation morphology independ on crystal orientation, and morphology related to stress deformation. The diamonds mainly belong to type IaAB and the nitrogen content in them is 22.90~752.40 μg·g^-1. The concentration of sp³ hybridized C—H bond is higher than of sp² hybridized C—H bond in most of the samples, that indicated the existence of hydrogen was conducive to transformation from the A nitrogen center to B nitrogen center in diamond and the sp³ hybridized C—H bond may result in the formation of corrosion pits and affect slightly the others morphology of the diamond surface. All of the surface morphologies would lower the degree of order of diamond. The degree of surface order was the highest in diamond with halo and the lowest in diamond with growth lamella.