Hexavalent chromium (Cr(VI)) is a heavy metal that is highly soluble and exhibits toxic effects on biological systems. Nevertheless, it is used in many industrial applications. The adsorption process of Cr(VI), using activated carbon (AC), is under investigation globally. On the other hand, around six million tons of spent coffee is sent to landfill annually. In the spirit of cyclic economy, this research investigated the production of AC from spent coffee for the removal of Cr(VI) from wastewater. The AC was produced via pyrolysis process under a nitrogen atmosphere. Chemical activation using potassium hydroxide (KOH) occurred simultaneously with the pyrolysis process. The produced AC was tested as an absorber of Cr(VI). The best fitted kinetic model was the diffusion–chemisorption model. A 24-h adsorption experiment was carried out using a solution with a pH of 3 and an initial Cr(VI) concentration of 54.14 ppm. This resulted in an experimental maximum capacity of 109 mg/g, while the theoretical prediction was 137 mg/g. It also resulted in an initial adsorption rate (ri) of 110 (mg/(g h)). The Brunauer–Emmett–Teller surface area (SgBET) was 1372 m2/g, the Langmuir surface area (SgLang.) was 1875 m2/g, and the corrugated pore structure model surface area (SgCPSM) was 1869 m2/g. The micropore volume was 84.6%, exhibiting micropores at Dmicro1 = 1.28 and Dmicro2 = 1.6 nm. The tortuosity factor (τ) was 4.65.