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A significant rise in the abuse of a new group of synthetic cathinones was reported recently in Western Europe. We selected four documented cases that recently occurred in Spain to discuss the toxicological significance and the mechanisms that explain the legal facts. All drugs and metabolites were detected using gas chromatography-mass spectrometry (GC-MS) and liquid chromatography-mass spectrometry (LC-MS-MS). Case 1: A 19-year old male was arrested for assaulting his father. He drank a random glass in a discotheque. He described a feeling of elation, irritability and several episodes of amnesia. Methylone and its metabolites, and 11-nor-9-carboxy-delta9-tetrahydrocannabinol (THC-COOH) were detected in urine. Case 2: A 33-year-old gay male committed suicide by hanging. Alpha-pyrrolidinovalerophenone (alpha-PVP) and 4-methylethcathinone were found in blood and urine. Cocaine and its metabolites were detected in urine. Case 3: A 53-year-old male went to the hospital suffering palpitations and thoracic pain and explained that he had inhaled a “white substance” while taking money from a cashier. The case was defined as drug facilitated crime (robbery). Alpha-PVP was detected in blood (0.009 mg/L) and urine, along with nordiazepam and lorazepam and metabolites. Case 4: The police restrained a 39-year-old Colombian male with agitation, persecutory psychosis and irrational behavior. Autopsy samples showed alpha-PVP in blood (1.20 mg/L) and urine along with cocaine, amphetamine, 3,4-methylenedioxy-methamphetamine, lormetazepam and alprazolam. The four cases bring attention to the severe toxicity including behavioral abnormalities induced by easily accessible synthetic cathinones, all of which should be taken into consideration by authorities in order to adjust legislation with celerity to real life circumstances.