When Two Dimensions Matter: A Critical Review of Recent Comprehensive Two‐Dimensional Gas Chromatography Applications in Food Analysis

Comprehensive two‐dimensional gas chromatography (GC×GC) is a powerful analytical technique for investigating the chemical complexity of food matrices by combining two complementary separation dimensions with mass spectrometric detection. Its enhanced separation capacity makes GC×GC particularly attractive for the characterization of volatile and semi‐volatile compounds, as well as for food authentication, quality assessment, contaminant determination, and comprehensive chemical profiling. This review critically examines several analytical applications of GC×GC in food analysis reported between 2021 and 2025, focusing on the problems addressed, the food matrices investigated, and the added value provided by two‐dimensional separation compared with conventional GC. A bibliometric analysis of publication trends, countries, and journals is combined with a systematic assessment of target compounds, sample preparation, column configurations, modulation systems, and detection strategies. Plant‐based foods were the most extensively investigated matrices, followed by animal‐based products and other food categories, while solid‐phase microextraction was the most frequently employed sample preparation approach. Attention is given to applications involving volatile compounds and aroma, foodomics, fingerprinting, authenticity, and contaminants. Finally, current limitations and emerging opportunities are discussed, highlighting the need for robust quantitative methods, improved data processing, and broader application of GC×GC to complex food matrices.