Natural clays have been recommended as a green alternative sorbent, with low cost, good mechanical properties, and good tolerance to a harsh chemical environment. However, on a large scale, it is difficult to separate the clay particles from the solution; the centrifugation process involves a high speed, and the filtration procedure is prone to filter blockages. Therefore, a suitable method for the separation of clay particles is necessary to be found. To solve this problem, the clay should be modified. In this paper, attapulgite (ATP) as a natural clay was modified using double-layer hydroxide to produce LDH-ATP sorbent. Different sorption isotherm models of the modified attapulgite for the removal of Sr²⁺, Co²⁺, and Ni²⁺ ions from a multicomponent solution were evaluated, for instance, the extended Langmuir and Freundlich isotherm models. The results demonstrated that the extended Langmuir is more suitable than Freundlich isotherm (with R² values greater than 0.95). The maximum capacity was computed and found to be 2.6, 1.64, and 1.60 mmol/g for Ni²⁺, Co²⁺, and Sr²⁺, respectively. Finally, the LDH-ATP can be recommended for the removal of Sr²⁺, Co²⁺, and Ni² ions from multicomponent media.