This study investigated the dynamic photo-response of pseudorotaxane crystals with azobenzene and ferrocenyl groups in the axle component. X-ray crystallography showed pseudorotaxanes with a methylazobenzene group and a dibromophenylene ring in the cyclic component to exhibit twisting of the trans-azobenzene groups at torsion angles of 17 degrees and 38 degrees, respectively. Repeated alternating laser irradiation of the crystals at 360 and 445 nm produced bending of 20-30 degrees in opposite directions, with no evidence of decay. Under 44S nm irradiation, bending took place within 0.3 s. A crystal of nonsubstituted pseudorotaxane showed bending of only 2 degrees under 360 nm irradiation due to multiple pi-pi interactions between the planar trans-azobenzene groups. The pseudorotaxane crystals have two chromophores, bent rapidly and reversibly on irradiation at rates depending on the molecular structure.