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Systematic toxicological analysis (STA) is an important step in medicolegal investigations of death, poisoning, and drug use. The primary goal is the detection and confirmation of potentially toxic compounds in evidence. This article describes a workflow using nontargeted liquid chromatography-tandem mass spectrometry (LC-MS/MS) for reliable compound identification. Tandem mass spectrometry was performed on a low-resolution quadrupole-quadrupole-linear ion trap instrument. Acquired spectra were submitted to automated library search, and positive matches were verified by expert reviewing. After validation, the nontargeted LC-MS/MS technique was integrated in the STA service provided by our laboratory. [ABSTRACT FROM AUTHOR]