In this work, Nd3+ was used as a surrogate and it was incorporated into Gd2Zr2O7 nanocrystalline ceramics to simulate the immobilization of trivalent actinide elements. A series of Gd2 − xNdxZr2O7 (0.0 ≤ x ≤ 2.0) nanocrystalline powders were fabricated by solvothermal method, and then Gd2 − xNdxZr2O7 sub-microncrystalline ceramics were prepared by sintering via self-propagating chemical furnace plus quick pressing (SCF/QP). All powders are in defective fluorite structure, and Nd doping hardly change the powder grain size. After analyzing the sintered ceramics, it can be found that the transition from defective fluorite structure to pyrochlore structure occurs when x ≥ 1.5. The sample density decreases with elevated Nd content, while the grain size gradually enlarges. Besides, the normalized release rates of Nd and Zr elements in the Nd2Zr2O7 waste form are kept in low values (below 10− 5 g•m− 2•d− 1), which exhibits its excellent aqueous stability.