The purpose of this paper is to summarize the most relevant and recent information available on ergot alkaloids. This includes information about their occurrence, toxicity, chemistry, statutory limits, and their significance in feed and food. Recently, in 2005, the European Food Safety Authority (EFSA) concluded that validated analytical methods for the quantification of ergot alkaloids in feed materials are needed. For that reason, the major focus of the present paper is to report on the latest developments for the determination of major ergot alkaloids and their epimers in cereals and cereal-derived products. Information about the stability and the availability of calibrants, sampling issues, extraction and clean-up strategies, and a variety of final separation and detection techniques is provided. The recently developed liquid chromatography-tandem mass spectrometric methods (LC-MS/MS) for the simultaneous quantification and identification of ergot alkaloids are given special consideration.