•An ASE-GC×GC–TOF/MS multiresidue method was set up for PAH analysis in food.•GC–MS/8O enabled a robust determination of odour zones.•Heart-cutting GC–GC–MS/O resolved the remaining coelutions of key odorants.•PAHs and odour-active compounds were investigated in cooked meat. The assessment of the dual impact of heating treatments on food safety and aroma is a major issue for the food sector. The aim of the present study was to demonstrate the relevance of multidimensional GC techniques, olfactometry and mass spectrometry for the parallel determination of process-induced toxicants and odorants in food starting with cooked meat as a food model. PAHs were analyzed by comprehensive two-dimensional gas chromatography-time-of-flight mass spectrometry after extraction by accelerated solvent extraction (ASE-GC×GC–TOF/MS). Odour-active compounds were determined by dynamic headspace–GC hyphenated with eightbooth olfactometry and mass spectrometry (DH–GC–MS/8O) and DH-heart-cutting multidimensional GC hyphenated with olfactometry and mass spectrometry (DH–GC–GC–MS/O). For PAH determination, the GC×GC conditions consisted of a combination of a primary non-polar BPX-5 column and a secondary polar BPX-50 column, and a modulation period of 5s. In terms of linearity (R2 ranging from 0.985 to 0.997), recovery rate (84–111%) and limit of detection (5–65ng/kg of cooked meat), the ASE-GC×GC–TOF/MS method was found consistent with the multiresidue determination of 16 PAHs including benzoapyrene in cooked meat. For aroma compounds, DH–GC–MS/8O and DH–GC–MS/O revealed 53 major meat odour-active compounds. A customized heart-cutting GC–GC–MS/O enabled the coeluting odour zones with high odour-activity to be resolved and revealed 15 additional odour-active compounds. Finally, these developments of multidimensional approaches were used to investigate the balance between 16 PAHs and 68 odour-active compounds generated with different cooking techniques.