The behavior of 16 volatile compounds of banana during a combination of air-drying (AD) and vacuum microwave-drying (VMD) of banana chips was characterized. Samples were AD to remove 60, 70, 80, or 90% of moisture (wet basis) and then subjected to VMD to achieve a final moisture content of 3% (dry basis). Banana slices were also dehydrated using only AD, VMD, and freeze-drying (FD) for comparison. Samples that underwent more VMD had significantly lower levels of volatile compounds, which is attributed to the decreased formation of an impermeable solute layer on the surface of the chips. High values for water solubility and relative volatility of compounds correlated with losses during VMD; however, additional factors appear to influence the behavior of compounds during VMD processing. The optimal process of 90%AD/10%VMD yielded crisper banana chips with significantly higher volatile levels and sensory ratings than AD chips.