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Previous research into the synthesis of urea-formaldehyde fertilizers was mostly based on orthogonal experimental designs or single factor tests; this led to low precision for synthesis and relatively large ranges of parameters for these processes. To obtain mathematical response models for the synthesis of urea-formaldehyde fertilizers with different nitrogen release properties, a central composite design (CCD) of response surface methodology was used in our research to examine the effects of different reaction times, temperatures, and molar ratios on nitrogen insoluble in either hot or cold water. Our results showed that nitrogen insoluble in cold or hot water from urea-formaldehyde fertilizers were mainly affected by urea: formaldehyde molar ratios. Also, quadratic polynomial mathematical models were established for urea-formaldehyde. According to the models, the optimal process parameters which maximize cold-water-insoluble nitrogen and minimize hot-water-insoluble nitrogen for the synthesis of urea formaldehyde were as follows urea: formaldehyde molar ratio was 1.33, reaction temperature was 43.5 °C, and reaction time was 1.64 h. Under these conditions, the content of coldwater-insoluble nitrogen was 22.14%, and hot-water-insoluble nitrogen was 9.87%. The model could be an effective tool for predicting properties of urea-formaldehyde slow release fertilizers if the experimental conditions were held within the design limits.