Increasing crop production and soil carbon sequestration is critical for sustainable agricultural development. Straw returning, a common agricultural practice, positively affects grain yield and soil organic carbon. Nevertheless, the slow decomposition rate and high carbon-to-nitrogen ratio of straw are significant obstacles to its effectiveness. Ammonifying straw using urea and calcium hydroxide may be a promising solution, whereas limited information is available on the impacts of ammoniated straw returning on crop production and soil carbon sequestration. Therefore, in a winter wheat-summer maize rotation system, we conducted an experiment with three straw returning treatments (T1, straw removal; T2, traditional straw returning; T3, ammoniated straw returning) to investigate their impacts on crop growth, grain yield and yield components, carbon inputs and outputs, and net ecosystem carbon budget (NECB). The results showed that T3 outperformed T2 regarding increasing leaf area index and aboveground biomass. Ear density and thousand kernel weight of winter wheat and hundred kernel weight of summer maize were ranked T1 < T2 < T3, with no significant differences between treatments for other grain yield components. Consequently, winter wheat, summer maize, and annual grain yields were the highest under T3, followed by T2 and T1. In comparison with T1, T2 and T3 increased annual total carbon inputs by 5463 and 7271 kg C ha–1, respectively, due to the increased carbon inputs from returned straw and net primary productivity. Annual carbon total outputs, primarily from aboveground biomass removal at harvest and carbon respiration, increased by 3305 kg C ha–1 under T2 and 4264 kg C ha–1 under T3, compared with T1. Balancing annual total carbon inputs and outputs, T1, T2, and T3 had annual NECB values of –1215, 944, and 1793 kg C ha–1, respectively. Therefore, the T1 agroecosystem acted as a carbon source, whereas the T2 and T3 agroecosystems, particularly T3, acted as a carbon sink on an annual scale. These results suggest that ammoniated straw returning may be a superior straw application practice for increasing crop production and soil carbon sequestration simultaneously.
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