Coffee is one of the most popular beverages, with around 10.5 million tons manufactured annually. The same amount of spent coffee grounds (SCGs) might harm the environment if disposed of carelessly. On the other hand, pesticide contamination in food and biowaste is a rising problem. Because pesticides are hazardous and can cause serious health consequences, it is critical to understand how they interact with food biowaste materials. However, it is also a question if biowaste can be used to remediate rising pesticide residues in the environment. This study investigated the interactions of SCGs with the organophosphate pesticides malathion (MLT) and chlorpyrifos (CHP) and addressed the possibility of using SCGs as adsorbents for the removal of these pesticides from water and fruit extracts. The kinetics of MLT and CHP adsorption on SCGs fits well with the pseudo-first-order kinetic model. The Langmuir isotherm model best describes the adsorption process, giving the maximal adsorption capacity for MLT as 7.16 mg g−1and 7.00 mg g−1for CHP. Based on the thermodynamic analysis, it can be deduced that MLT adsorption on SCGs is exothermic, while CHP adsorption is an endothermic process. The adsorption efficiency of MLT and CHP using SCGs in a complicated matrix of fruit extracts remained constant. The neurotoxicity results showed that no more toxic products were formed during adsorption, indicating that SCGs are a safe-to-use adsorbent for pesticide removal in water and fruit extracts.