To solve the problem of drying gelcast green body, the thermoresponsive gel system which contains macromonomer graft chains was used in gelcasting of ZnO. The effects of the amount and length of graft chains macromonomer PIPAAm, the total amount of organic matters, and the solid loading on the rheological properties of suspensions were investigated, and the drying mechanism of gelcast green body was analyzed. The results show that ZnO suspensions with the gel system still display shear-thinning rheological behavior, but its viscosity increases with increasing the addition amount and relative molecular mass of PIPAAm graft chain, and the total organic matter content. The PIPAAm graft chains inhibit or even eliminate the formation of the “dense layer” on the surface of gelcast ZnO green bodies, and accelerate the drying of green bodies. The introduction of PIPAAm graft chains facilitates the shrinkage of the gelcast ZnO green bodies, which is a feasible method to increase the relative density of green bodies.