This research investigated methods for tailoring a commercial, lignite-based granular activated carbon (GAC) to enhance its adsorption of 2-methylisoborneol (MIB) from natural water. Tailoring efforts focused on heat treatments in gas environments comprising steam and/or methane, since these gases can alter GAC pore structure and surface chemistry. Heat treatments that combined methane and steam enhanced MIB adsorption considerably, causing a 4-fold improvement (over untreated GAC) in fixed-bed adsorption performance relative to initial MIB breakthrough. These favorable effects, observed in rapid small-scale column tests, occurred following simultaneous and separate (sequential) applications of methane and steam. Moderately low temperature steam treatments also improved MIB uptake in fixed-bed adsorption tests but to a lesser extent (approximately 1.5-fold). In contrast, methane treatments alone, at various temperatures, led to significant carbon deposition within the GAC pore structure. As a result, total pore volume was reduced and MIB adsorption performance declined.