Pyramids/particles of NiO/SnO2 composite (NS7) was produced by applying the sol–gel autocombustion method. The produced composite was investigated using different techniques, X-ray diffraction, Fourier-transform infrared, Raman spectroscopy, scanning electron microscope, dynamic light scattering, ultraviolet–visible absorbance spectroscopy, and BET surface area then was applied for the adsorption and separation of molybdenum and zirconium ions from lanthanum, strontium, and cesium. 3D pyramids of NiO and particles of SnO2 are confirmed in the composite with a homogeneous mesoporous structure. The composite has good affinity for zirconium and molybdenum ions with fast kinetics and Qmax of 27.1 and 33.3 mg/g, respectively, low affinity for lanthanum, and negligible affinity for strontium and cesium. The sorption mechanism is physical sorption and endothermic in nature. The adsorbed Zr(IV), Mo(VI), and La(III) ions were separated using the desorption process as the following sequence: First, 95 ± 2% (14.3 ppm) of the loaded La was desorbed by washing with double distilled water. Then 96 ± 2% (41.3 ppm) of the loaded Zr was recovered by 1 M potassium chloride without interfering ions. Finally, 98 ± 2% (42.88 ppm) of Mo is desorbed by 1 M sodium acetate solution. The NS7 composite can be reused five times successfully.