Urea or biuret was added to the thermal synthetic system of Rhabdophane-type neodymium and cerium phosphates. The mixture of a rare earth compound, a phosphorus compound, and an additive [CO(NH2)2 or NH(CONH2)2] was heated at 150°C or 300°C for 20 hr, and the thermal products were analyzed by the XRD, FT-IR, and BET methods. H3PO4 and (NH4)2HPO4 were used for phosphorus compounds, and for rare earth compounds, Nd2O3, Nd(NO3)3 · 6H2O, NdCl3 · 6H2O, Nd2(CO3)3 · 8H2O, CeO2, Ce(NO3)3 · 6H2O, CeCl3 · 7H2O, and Ce2(CO3)3 · 8H2O were used. Urea and biuret worked not only as a dispersing agent but also as a reactant. By the addition of biuret, the thermal products changed from cerium oxide to Rhabdophane-type cerium phosphate in the system using CeCl3 · 7H2O and (NH4)2HPO4. Addition of urea or biuret influenced the specific surface area of Rhabdophane-type neodymium and cerium phosphates. Furthermore, to increase the reactivity of the raw solid materials, mechanical treatment was performed. The mixture of diammonium hydrogenphosphate and a rare earth compound was ground with water and then heated. The influence of the addition of urea or biuret was also studied in these systems.