Abstract A reliable supply of nitrogen is essential for agricultural productivity, and therefore meeting global food demands. However, the management of nitrogen for sustainable development remains challenging, and this situation is likely to worsen due to the combined effects of land degradation, anthropogenic climate change, and rapid population growth. Furthermore, the escape of reactive nitrogen form agricultural soils has adverse implications for human and environmental health. Therefore, if we are to increase crop productivity whilst mitigating the adverse effects of reactive nitrogen in the environment, it is important to have a detailed molecular-scale understanding of the forms and turnover of nitrogen in soil as a prerequisite to improving global nitrogen-use efficiency. This data article combines the application of High-Resolution Magic Angle Spinning (HR-MAS) NMR spectroscopy and allied analytical approaches to provide molecular-scale understanding of the forms and dynamics of organic nitrogen in soils, using microbial-derived proteins as a surrogate.