Soil organic nitrogen (SON) components are a key indicator of soil fertility and plant growth. The Danxia degraded region (DDR) is an ecologically fragile area in southern China, where the “Grain for Green” project has been implemented to prevent further land degradation. However, little is known about the effects of vegetation restoration on SON components in the DDR or the factors that influence them. We compared three vegetation restoration types, namely, grassland, shrubland, and arbor forest, with cropland to determine the relationship between SON components and N−cycling enzyme activities. Vegetation restoration increased the soil amino sugar N and amino acid N and reduced the proportion of non−hydrolyzable N. Compared with forest restoration measures, restoration to grassland was more beneficial to SON levels and N−fixation capacity. Vegetation restoration also increased soil nitrate reductase, denitrifying enzyme, protease, β−1,4−N−acetylglucosaminidase activities, and soil microbial biomass. Vegetation restoration in the DDR changed the SON components through the “mineralization−fixation” of organic matter via amorphous iron and proteases, which, in turn, affected the level of available soil N. Vegetation restoration improved the soil N structure and promoted the intrinsic soil N cycle, providing a scientific basis for soil quality restoration in the DDR.