Phase transformation and bloating behavior of novel CaMgSi2O6 glass-ceramics with ZrO2 nucleating agents, prepared using two-stage heat treatment; were investigated and evaluated as microwave dielectric materials. Experiments show that specimens annealed below critical nucleation temperature (Tcn) and sintered at 950oC reveal significant bloating phenomena. Kinetic study of CaO-MgO-SiO2-ZrO2 (CMSZ) glass annealed below Tcn reveals high activation energy of crystallization for ZrO2 nucleation, and zirconia dissolved into CMSZ glass and formation of fleeing oxygen can be attributed to sluggish crystallization of ZrO2 agents. On the other hand, specimens of CMSZ glass annealed above Tcn, microstructural features exhibit that zirconia precipitated significantly in the CMSZ glass at beginning, and then are accompanied by the rapid growth of CaMgSi2O6 phase around the ZrO2 crystallites, indicating enhanced crystallization of nuclei due to growth over the critical size of nuclei at an annealing temperature above Tcn. In addition, specimens using two-stage heat treatment and annealed above Tcn reveal much higher densification properties as microwave dielectric materials.