A rare example of a novel zeolite-induced conformational change and a mechanism for this process are suggested in order to rationalize an unexpected spontaneous intrazeolite reduction observed during preparation of a new viologen (MQ(2+))-doped zeolite (NaY). In addition, the formations of six new alkene/viologen/ zeolite charge transfer (CT) arrays using NaMQY and the previously reported NaMVY are also reported. The binding constants between MQ(2+) and MV2+ and 2,3-dimethyl-2-butene (TME) were determined using the Benesi-Hildebrand approach, and the stabilities of these CT complexes are compared to their intrazeolite analogue.