The pristine 2D bilayer COF was prepared with boroxine (B 3 O 3 ), triazine (C 3 N 3 ), and benzene (C 6 H 4 ) rings. It was built using two layers with P6m2 symmetry (space group 187). In the unit cell, each COF layer is comprised of one triazine, one boroxine, and three benzene rings, and the two layers are stacked directly on top of each other (eclipsed stacking). The reason for this combination of building units is to maximize the environment of different TM atoms and organic rings, while maintaining synthesis feasibility which can explore the effects of TM atoms in the different rings. Seven different types of TM-intercalated 2D bilayer COFs were computationally prepared through the addition of TMs at the centroid of the bilayer COF rings: