Although several methods exist for the synthesis of circularly polarized luminescent (CPL) materials, the methods are extremely complex and tedious. In recent years, the chiral host-achiral luminescent guest method and the achiral host-achiral luminescent guest method have been employed to fabricate CPL materials; however, the main disadvantage of the latter is the small luminescence dissymmetry factor (glum) that limits the practical applications of the method. Therefore, this study reports on the enhancement of glum in a nano-segregated phase system, generated by the phase separation between helical nanofilaments (HNFs; originating from an achiral bent-core molecule) and a liquid-crystalline (LC) smectic A (SmA) phase (originating from an achiral rod-like mesogen). The observed glum value in the nano-segregated phase between the HNFs and LC SmA phase was larger than that in the nano-segregated phase between the HNFs and LC nematic (N) phase. The enhancement of the glum value was attributed to the order parameter (S) of the dye molecules in the SmA phase being larger than that in the N phase. Therefore, we concluded that the S value of the fluorescent dye molecules, doped into the embedded LC phase between the HNFs, strongly influenced the glum value.