Efficient negative photochromism was achieved by the photoinduced migration of merocyanine in mesoporous silica to an organophilic clay as spiropyran. Depending on the nature of the organophilic clays (dioctadecyldimethylammonium and dioleyldimethylammonium clays), important differences in the negative photochromisms and the thermal coloration were observed; the dioleyldimethylammonium clay gave a higher yield (98%) and faster reaction (half-life t1/2 = 2.8 h) than the dioctadecyldimethylammonium clay (94% and t1/2 = 3.2 h) of the negative photochromism, indicating the important role of the surfactant assembly to control the molecular diffusion.