Methyleugenol is a substance that is possibly carcinogenic to humans, which may occur in foods containing certain herbs and spices. The European Union has set maximum levels for some product groups, but there is a lack of comprehensive market surveys for this compound. In this study, we compare two procedures for methyleugenol determination in foods, namely GC/MS, which is currently seen as gold standard for such an analytical problem, and NMR, which is hypothesized to be suitable as a faster screening. The sample preparation for GC/MS consists of homogenization in ethanol followed by liquid–liquid extraction for fat-free foods or automatic steam distillation for fat-containing foods. The extract or distillate is then measured using GC/MS either in SCAN or SIM mode (dependent on concentration) with cyclodecanone as internal standard. For 1H NMR, the ethanolic solution can be directly measured without further extraction or distillation. Quantification using external standardization is conducted for NMR. Both procedures were validated and fulfilled the requirements for quantitative food analysis. The applicability was demonstrated by analyzing 120 samples including basil, estragon, pimento, nutmeg, several teas, alcoholic beverages, and pesto. GC/MS is more sensitive, precise, and suitable for regulatory purposes but time-consuming and expensive. NMR can be used for a faster screening analysis and appears to be ideal for conducting larger surveys to estimate human exposure.