The kinetics of tetragonal Nd2Si2O7 crystallization from polymeric xerogels was investigated under non-isothermal conditions via differential thermal analysis (DTA). The polymeric xerogels were prepared by the Pechini sol-gel method from tetraethoxysilane and neodymium nitrate. The crystallization fraction and rate of tetragonal Nd2Si2O7 were determined based on the exothermic DTA data. The activation energy of tetragonal Nd2Si2O7 crystallization, which is calculated by the Kissinger equation, is 673 kJ/mol. The crystallization process of tetragonal Nd2Si2O7 could involve the nucleation and three-dimensional growth that follows the diffusion-controlled mechanism when the nucleation rate increased.