The solubility of 1-methyl-3, 4, 5-trinitropyrazole (MTNP) in different solvents was determined by the gravimetric method. The Apelblat equation and vant′t Hoff equation were used to correlate the solubility data. The standard enthalpy of dissolution, standard entropy of dissolution, standard Gibbs free energy of dissolution, solid-liquid surface tension and surface entropy factor of MTNP were estimated by the experimental data. By comparing the solubility data of MTNP, benzene, methanol and ethanol absolute were used to crystallization as solvent and the product was characterized. Results show that the solubility of MTNP increases with increasing the temperature. The mean absolute percentage deviation between the fitted and experimental values of the Apelblat and vant′t Hoff equation is less than 5.18%, but the experimental data correlated by the Apelblat equation is superior. The morphology of the product crystallized using ethanol absolute observed by electron microscopy is regular and uniform. The impact sensitivity of product crystallized by ethanol absolute is 68%. The size uniformity of product measured by the BT-2002 laser particle size analyzer is better.