The molecular structures of our targeted molecules are provided in Figure . Polycyclization decoration on the central ring of the well-known (DtBuCzB) has been a reported strategy to not only modulate emission spectra but also disrupt peripheral symmetry to construct helicene structures for chiral emission. Our molecular also adopted this strategy by fusing an indolo and N-hetero[8]helicene structure, those two decoration segments were also wisely chosen considering that, on one hand, different to the usually adopted non-MR polycyclic aromatic hydrocarbons, both emitters possess MR characteristics and thus the orbital distribution extended to them would also maintain the MR characters, which favors keeping a narrowband emission. On the other hand, two segments bear opposite electronegativity and thus the different charge distribution can be anticipated for two emitters, which allows us to study the influence on CPL properties from an electronic-level insight given their similar geometrical structures. The molecular here therefore not only enriches the molecular design discourse but also may deepen the understanding of the interplay between structure and chiroptical behaviors.