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Rhabdophane has been considered an important permeable reactive barrier to isolate groundwater radionuclides, and evaluating its precipitation response to different species of radionuclide in acid solutions is critical. In this work, the effects of pH values on the precipitation behavior of Nd3+ and Sm3+ into La-rhabdophane are systematically investigated. Some specific issues such as ions removal, precipitation reaction kinetics, and crystal growth affected ions incorporation are discussed in detail, along with uncovering the veil of the Ln (La, Nd, and Sm) leaching mechanism of associated La0.666Nd0.167Sm0.167PO4 monazite ceramic based on dissolution experiments and density functional theory. The results reveal that Nd3+ and Sm3+ can be removed more than 98% in pH = 1 solution within 12 h, whereas uneven precipitation process to form unexpected stoichiometric ratio of rhabdophane has been observed in 30-50 nm short crystal. Grain growth effects based on spark plasma sintering can contribute to homogenize the materials composition with obtaining La0.666Nd0.167Sm0.167PO4 monazite ceramics. Furthermore, the binding energy of Ln-O in (1 0 0) surface of monazite plays an important role in controlling the leaching stability of Ln(3+), associated with the leaching activities are energetically favorable in the order of La > Nd > Sm for La0.666Nd0.167Sm0.167PO4 monazite.