Photochromism of 1,2-bis(2,5-dimethyl-3-thienyl)perfluorocyclopentane (1a) and 1,2-bis(2-methyl-6-nitro-1-benzothiophen-3-yl)perfluorocyclo-pentane (2a) in single-crystalline phases was investigated. Upon irradiation with 366 nm light the colorless crystals of la and 2a turned red and green, respectively. The colored crystals are due to the formation of the closed-ring isomers, Ib and 2b, The colored crystals were breached by irradiation with visible light. The direction of the electronic transition moment of 1b in crystal was estimated from the absorption anisotropy of 535 nm band. When the photogenerated green colored crystal of 2a was observed under polarized light, the colored crystal showed dichroism of yellow and blue. The yellow and blue colors were attributed to two perpendicular electronic transitions of 2b at 465 and 600 nm, respectively.