Chirality has been an important subject in chemistry since Pasteur demonstrated the existence of molecules that were mirror images of each other. [1] Indeed, chirality has proven to be important in the fields of biology and pharmacy as well. [2] In the past, single enantiomers have been made by using asymmetric catalysis [3,4] and enantiomeric separation. [5] However, almost all methods rely on the use of chiral molecules. Recently, the development of asymmetric reactions that do not use chiral molecules is attracting lot of attention. In this respect, bent-core liquid crystals (BCLCs) [6][7][8] are very interesting because layer chirality occurs in nonchiral molecular systems as a result of the tilt of polar-ordered molecules from the normal of the smectic layer, [9] and is coupled with conformational molecular chirality. [10] Moreover spontaneous deracemization to give large chiral domains occurs particularly in the helical nanofilament (HNF) B4 phase because of negative splay elastic constants. [7][8][9][10][11][12] Each macroscopic chiral domain consisting of HNFs exhibits high optical activity. [11,[13][14][15] The formation of a helical structure in the B4 phase suggests that the chirality can be controlled, because in many other organic systems the handedness of the helical structure has been controlled by external chiral sources, such as circularly polarized light, [16,17] vortex flow, [18][19][20] and helicity memory induced by chiral molecules. [21] Previously, we used five different methods to control the chirality of the B4 phase and successfully obtained almost 100 % ee with some of them. These methods are: 1) the introduction of chiral analogues, [22] 2) the use of a chiral surface, [23] 3) irradiation of photoisomerizable molecules with circularly polarized ultraviolet (UV) light, [24] 4) the use of twisted nematic (TN) director orientation, [25] and 5) growth from a chiral phospholipid layer. [26] Methods 2 and 5 both involve the use of a chiral surface, however, with the former only 10 % ee was attained, whereas with the latter almost 100 % ee was attained. The difference originates from the absence (method 2) and presence (method 5) of a temperature gradient. Contrary to the use of chiral dopants in method 1 and chiral surfaces in methods 2 and 5, methods 3 and 4 do not require any chiral species and have the added advantage that they work on bulk samples. However, the phase sequences of the compounds used for methods 3 and 4 are restricted by necessary phase sequences, that is, a fluid smectic phase (method 3) and a nematic (N) phase (method 4) that occur at higher temperatures to the B4 phase. Namely, a gradual phase transition from fluid smectic phases to the B4 phase under circularly polarized UV irradiation triggers repeated photoisomerization, whereas UV irradiation in the B4 phase is not an effective method to control chirality. Only one example of method 4 is known [25]