In recent years, practical, inexpensive, and highly specific electroanalytical methods based on modified electrodes have been increasingly developed for forensic science. Simple modification of the carbon paste electrode with Schiff base complexes has become a promising strategy to detect and quantify narcotics. In this context, we aimed to develop voltammetric methods to quantify lysergic acid diethylamide (LSD) by using a carbon paste electrode modified with the complex [UO2(Ac-ophen)]·H2O. The use of an aqueous solution of KCl as supporting electrolyte makes the methodology less polluting, which contrasts with methods that still employ toxic solvents. The developed method for Differential Pulse Voltammetry provides a linear response at various concentrations of LSD and affords analytical curves with standard deviation, detection, and quantification limits around 2.45, 0.625, and 2.08 μmol L-1, respectively. The recovery values of 103 and 108% prove that the developed method is suitable for application in forensic science.