The effect of nickel in the adsorption of N-acetyl-p-aminophenol (paracetamol) on a metal-organic frameworks (MOFs) type MIL-101(Cr) was studied. The incorporation of Ni to MOFs adsorbent was carried out by impregnation and adjusted to give a 4.00 wt.% Ni. The adsorbents were characterized by specific surface area (SSA), surface acidity techniques, electrophoretic migration (EM), thermogravimetric analysis (TGA), and scanning electron microscope (SEM) and were tested by the adsorption of paracetamol solutions. The results showed that the Ni particles were well dispersed throughout the MIL-101(Cr) crystal increasing the acid strength and the density of acid site values in the MOFs surface. The increase in adsorption capacity of MIL-101(Cr) when Ni was incorporated can be attributed to the availability of metal atoms as adsorption centers that can adsorb the paracetamol by electronic retro-donation through π-type complexing.