This work analyzes the synergy between two complementary unit operations - adsorbent dehumidification and drying - and presents a mixed integer nonlinear programming approach to optimize energy performance in a two-stage system. Combined with active constraint analysis, the adsorbent properties that promote energy performance are derived. Microporous adsorbents with higher sorption capacities at low vapor pressures and requiring higher regeneration temperatures are preferred for ambient air dehumidification in the first stage. For exhaust air dehumidification, mesoporous adsorbents with lower regeneration temperatures are preferred such that the exhaust air from the first regeneration stage can sufficiently regenerate them. For drying below 50 C, energy consumption reductions of about 70% are achieved compared to conventional dryers without adsorbent dehumidification depending on adsorbent properties. The results demonstrate the usefulness of superstructure optimization in matching the drying process with the capabilities of the adsorbents to enhance process synergy for improved energy efficiency. © 2013 American Chemical Society.