Molybdenum (VI) oxide nanoparticles (α-MoO3 NPs) were green synthesised using buckthorn leaf extract as the reducing and capping agents. The α-MoO3 NPs were characterised by thermogravimetric analysis, fourier transforms infrared spectroscopy, X-ray diffraction, field emission scanning, and transmission electron microscopy, energy-dispersive x-ray spectroscopy, and Brunauer–Emmett–Teller surface area analysis. The analyses showed the formation of spherical-shaped α-MoO3 NPs with ∼50 nm mean crystallite size, 3.825 m2 g-1 surface area, and 0.005 cm3 g-1 total pore volume. The synthesised α-MoO3 was then applied for adsorption of Cd (II) from aqueous solutions. Optimisation of various adsorption parameters resulted in complete Cd (II) removal under the conditions: 0.1 g α-MoO3 dose, 60 min contact time, 50 mg l-1 initial Cd (II) concentration, pH 7 and 298 K. The experimental results were further assessed using different kinetic, isotherm and thermodynamic models. The data were best described by pseudo-second-order (R2 = 0.992) and Langmuir (R2 = 0.98) models with a maximum adsorption capacity of 57.5 mg g-1 at optimum conditions. Thermodynamic results indicated that the adsorption process is feasible, spontaneous, and endothermic in nature. Moreover, upon regeneration and interference results, α-MoO3 is stable and selective for Cd (II) adsorption in presence of other cations. Upon these results, the biosynthesised α-MoO3 NPs can be used as a selective adsorbent for the efficient removal of Cd (II) from aqueous media.