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Anthropogenic deterioration of the global nitrogen (N) cycle emerges mainly from overuse of inorganic N fertilizers in nutrient-limited cropping systems. To counteract a further dysregulation of the N cycle, we need to improve plant nitrogen use efficiency. This aim may be reached via unravelling all plant mechanisms to access soil N, with special attention to the dominating high-molecular-mass N pool. Traditionally, we believe that inorganic N is the only plant-available N pool, however, more recent studies point to acquisition of orga