Al2O3-poly(vinyl alcohol) nanocomposite (Al2O3-PVA nanocomposite) was generated in a single step using an eco-friendly method based on the pulsed laser ablation approach immersed in PVA solution to be applicable for the removal of Ni(II) from aqueous solution, followed by making a physicochemical characterization by SEM, XRD, FT-IR, and EDX. After that, the effect of adsorption parameters, such as pH, contact time, initial concentration of Ni(II), and medium temperature, were investigated for removal Ni(II) ions. The results showed that the adsorption was increased when pH was 5.3, and the process was initially relatively quick, with maximum adsorption detected within 90 min of contact time with the endothermic sorption process. Moreover, the pseudo-second-order rate kinetics (k2 = 9.9 × 10−4 g mg−1 min−1) exhibited greater agreement than that of the pseudo-first-order. For that, the Ni(II) was effectively collected by Al2O3-PVA nanocomposite prepared by an eco-friendly and simple method for the production of clean water to protect public health.