Comprehensive two-dimensional gas chromatography (GC.GC) is a powerful analytical tool that can be applied to food and essential oil samples to enhance separation capacity and spectral resolution capabilities. This analytical technique also allows better peak identification assignments when used in tandem with spectrometric detection systems by means of fewer interferences and thus true mass spectra of the individually isolated compounds in the 2D space. The development of more accurate and sensitive quantification methodologies permit improved characterization of complex samples, or target compounds in complex matrices. New approaches to isolation of aroma compounds from the matrix, for olfactory assessment based on targeted multidimensional GC are possible.