Water bodies face persistent contamination from organophosphorus pesticides like chlorpyrifos and malathion, which pose substantial environmental and health hazards due to their toxicity and resilience in ecosystems. This study explores the potential of spent coffee grounds, a common agricultural byproduct, as an eco-friendly adsorbent for eliminating these pesticides from polluted water. Spent coffee grounds underwent carbonization at 400 °C and various activation treatments using KOH, H3PO4, CO2, and their combinations. The impact of these activation methods on the adsorption capacity of carbonized materials was assessed under environmentally relevant conditions (25 °C, pH=6, and typical pesticide concentrations in wastewater). Results revealed that the physical and chemical properties of biowaste-derived materials significantly influence their adsorption efficiency, with KOH-activated adsorbents exhibiting the highest capacities ((16.1 ± 0.8) mg g−1 for chlorpyrifos and (11.2 ± 0.2) mg g−1 for malathion). Spent coffee grounds carbonized at 400 °C without additional activation demonstrated similar adsorption performance to the best-performing material ((19.4 ± 0.4) mg g−1 for chlorpyrifos and (10.6 ± 0.4) mg g−1 for malathion), with notably lower economic and environmental costs. Given its straightforward preparation and significant adsorption capacity, this material stands out as a sustainable solution for treating agrochemical wastewater containing chlorpyrifos and malathion.