An integrated system having the combined capability to perform gas chromatography (GC), comprehensive two-dimensional GC (GC X GC), and target heart-cut multidimensional GC (MDGC) using olfactometry (O), flame ionization (FID), and/or mass spectrometry (MS) detection is described. This combines a number of contemporary GC methods into a single instrument to provide very high resolution profiling of a sample. This provides initial assessment of volatile compound composition through GC X GC analysis with FID, which can be correlated with GC analysis using parallel O and FID detection. Subsequent microfluidic (Deans) switching selects regions (heart-cuts) of the chromatographic elution from the first dimension (1D) column for further resolution on a long second dimension (2DL) column for parallel detection of O and MS. Various 2DL operational conditions, as well as the effect of different heart-cut (H/C) duration, were compared. The favored mode involves cryotrapping of heart-cuts, cooling the oven, and reducing carrier flow to offer greater efficiency. An analytical strategy that incorporates GC-FID/O, GC X GC-FID, and MDGC-MS/O analyses with cumulative solid phase microextraction (SPME) sampling for volatile sample enrichment is presented in this work. Excellent qualitative and quantitative performance was demonstrated with a Shiraz wine sample and an allergens mixture, with tentative identification of acetic acid, octen-3-ol, and ethyl octanoate as aroma contributors in Shiraz wine and determination of beta- damascenone (floral odor) well separated from hexanoic acid (sweaty odor). A novel approach to obtain 2D retention indices is reported, allowing matching of mass spectral, 1I (retention index in 1D) and 2I (retention index in 2D) data. The method employs the same olfactory detector at the end of the 1D and 2DL columns.