Zircon (ZrSiO4) ceramics are candidate waste form for immobilizing actinides. However, ZrSiO4 with single phase suffers from the low actinides solubility. Herein, 0.2Zr1-aNdaO2-a/2/Zr1-bNdbSiO4-b/2 (0≤a+b ≤ 0.3) multiphase ceramics were fabricated and their actinides immobilization ability and aqueous stability were evaluated. The evolutions of phase and microstructure affected by Nd doping were investigated. 0.2Zr1-aNdaO2-a/2/Zr1-bNdbSiO4-b/2 ceramics with 0≤a+b˂0.1 exhibited monoclinic ZrO2, tetragonal ZrO2 and ZrSiO4 mixed phases, while monoclinic ZrO2, tetragonal ZrO2, ZrSiO4 and Nd2Si2O7 phases with 0.1≤a+b ≤ 0.3. The increase of lattice volume revealed the successful lattice immobilization of Nd by ZrO2/ZrSiO4. Due to synergistic immobilization effect, the Nd immobilization capacity of ZrO2/ZrSiO4 is up to 10 at%, which is higher than that of single-phase ZrSiO4 (4 at%). Furthermore, the obtained ceramics waste form exhibited good compactness and excellent aqueous stability. The results indicated that zirconia/zircon multiphase ceramics can be a potential candidate waste form for actinides.