With growing concerns regarding environmental pollution and the need for sustainable waste management practices, this study investigates the potential of utilizing spent coffee grounds (SCG) as a precursor for producing functional carbon materials aimed at organophosphorus pesticide remediation under environmentally relevant conditions. Carbonization of SCG is followed by various activation methods, including treatment with potassium hydroxide, phosphoric acid, and carbon dioxide, individually or in combination. The resulting biochars are systematically analyzed for their adsorption performance towards malathion and chlorpyrifos. Screening tests revealed a selective adsorption preference towards aromatic chlorpyrifos over aliphatic malathion. Activation processes significantly influence adsorption kinetics and efficiency, with physical activation showing notable adsorption rates and capacity enhancements. Moreover, the SCG-derived biochars exhibit a pronounced dependency on adsorption temperature. Adsorption, regeneration, and reuse of the most promising material are tested in a real, spiked tap water sample, proving that the presence of ions in tap water did not affect the adsorption and that the material has the potential to be reused more than ten times. This work proposes a straightforward approach for recycling SCG by converting it into functional carbon materials, underscoring the importance of selecting the appropriate activation processes and conditions for practical applications in pesticide remediation.