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It is thus essential and critical to enhance phosphorus (P) fertilizer use efficiency of crops to improve agricultural and environmental sustainability. A pot experiment was conducted to examine the impact of different kinds of value-added P-potassium (K)-activator fertilizers (VPAFs) on soil nutrient bioavailability, growth and yield of wheat-maize crops. Compared with that of the control (NPK) treatment, the wheat yields of VPAF treatments increased from 6.59% to 18.61%, and the maize yields increased from −0.22% to 15.58%. In addition, the P fertilizer utilization rate of VPAF treatments increased by an average of 10.87% and 5.75% for wheat and maize, respectively. Therefore, VPAF application in agriculture can introduce multiple benefits including increasing crop yield, improving fertilizer utilization efficiency, enhancing nutrient bioavailability, and reducing pollution.