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In response to the low separation efficiency of actinide nuclide (An) and fission product (FP) in the separation process of high‐level radioactive waste, as well as the large amount of secondary waste. A novel Ln(1‐x)SrxZrO(3.5‐0.5x) (0 ≤ x ≤1) multiphase ceramic waste form (Nd3+ simulating An3+), which can cure both An and Sr simultaneously, was in‐situ synthesized by sol‐gel spray pyrolysis method. The series of multiphase ceramics are composed of cubic pyrochlore phase Nd2Zr2O7 (NZO) and orthorhombic perovskite phase SrZrO3 (SZO), without any accompanying impurities. The two phases exhibit excellent compatibility, and their content can change regularly with the change of x. Nd and Sr occupy their most stable crystal lattice positions, with low transposition doping levels. The density of the composite ceramics is high, and the measured density is as high as 88 % of the theoretical density. The above experimental results confirm that the new multiphase ceramics can cure An and Sr simultaneously and separately, showing strong adaptability to waste components and high chemical stability. [ABSTRACT FROM AUTHOR]