In this section, we highlight the electronic properties of our intercalated 2D COF bilayers. Our main initial hypothesis was that, by changing the type of transition metal and its concentration, it is possible to fine-tune the bilayer COFs' electronic properties. Table columns 4-7, show the spin-polarized bandgap values and their type (direct, indirect, conductor) for all 2D COFs calculated in this work. As an initial observation, some of our materials (Co-01a/b, Co-03, Co-05, Cr-01a/b, Cr-04a, Cu-01a/b, Cu-03, Cu-05, Fe-03, Fe-04b, Fe-05, Ni-03, Ni-04a/b, Ni-05, Sc-01a/b, Sc-04b, Ti-01a, Ti-02, and Ti-05) have conducting electronic behavior in at least one of their spin channels. Therefore, our studies confirm that intercalation can be used to enhance the conductivity of these materials. This is a drastic change from the pure 2D COF, which presented insulating behavior (3.40 eV bandgap) and significant energy gaps below the Fermi level. The data in Table also indicates that most of our 2D COFs are semiconducting; moreover, our spin-polarized calculations reveal that most of these materials have different bandgaps for α(spin-up) and β (spin-down) states. To further explore the intercalated 2D COFs' electronic properties, we plot the band structures and DOS of all intercalated structures aligned with respect to vacuum. These plots can be found in the Supplementary Information (Figures ). Through these plots, we observe a general trend where the addition of TMs in the structure reduces not only the bandgap, but also the electron density gaps within the structures (below the valence band minimum). We will further expand on how this affects the potential applications of these materials in the following subsections.