In a wheat/maize rotation system, nitrogen (N) accounts for a large proportion of basal fertilizer, but soil N loss and the resulting environmental risk simultaneously exist worldwide. This study applied different urease/nitrification inhibitors together with basal fertilizers and investigated their effects on soil N level and grain yield. Six N stabilizing combinations consisted of two urease inhibitors (HQ and NBPT) and three nitrification inhibitors (DCD, DMPP, and Nitrapyrin). The treatments supplied with urease/nitrification inhibitors reduced, to some degree, the conversion rate of into , and kept content higher in surface soils for a longer time. Compared to CK, A1 treatment supplied with 1.5% HQ + 4% DCD well-maintained the levels of soil alkali-hydrolyzable N and . For example, alkali-hydrolyzable N and contents at 0–20 cm soil layer under A1 were increased by 8.59–41.6% and 8.15–14.5% more than CK, respectively. Based on the entire growth period of wheat and maize rotation, urease/nitrification inhibitors improved soil available N in surface soils but did not prevent and leaching, especially in the intensive rainfall season. The combinations of HQ and DCD or Nitrapyrin significantly enhanced crop yield. Specifically, crop yields under A1 and A3 (1.5% HQ + 0.25% Nitrapyrin) were 16.3% and 14.3% higher than CK, respectively. The N stabilizing combinations also promoted N intake and transport at every growth stage. The maximum N accumulation was increased by 27% under A1, when compared to CK. The treatments supplied with urease/nitrification inhibitors also achieved higher apparent N recovery efficiency, N agronomic efficiency, and N partial factor productivity. Consequently, the combinations of urease/nitrification inhibitors could improve N availability at 0–40 cm soil layer, which in turn improved N use efficiency of wheat and maize. The results suggested that the two urease/nitrification inhibitor combinations, 1.5% HQ + 4% DCD (A1) and 1.5% HQ + 0.25% Nitrapyrin (A3), were optimal N stabilizing agents and worthy of further study.