From Table , we also observe that eighteen of our compounds are semiconducting/insulating in one of their spin channels and conducting in the other, i.e., they present half-metallic behavior (Co-03, Cr-01a, Cr-01b, Cr-04a, Cu-01a, Cu-01b, Fe-04b, Fe-05, Ni-03, Ni-04a, Ni-04b, Ni-05, Sc-01a, Sc-01b, Sc-04b, Ti-01a, Ti-02, Ti-05). Due to their conductivity in only one spin orientation, half metals have applications in spin-based electronics, for example, as spin-injectors 39 in spin-based transistors and diodes. Three of these compounds (Cr-04a, Fe-04b, and Ni-04a) have a direct bandgap in their conducting channel, while the rest are indirect. The half-metal bandgaps range from 0.52 eV to 3.58 eV in their semiconducting/insulating channels, with several intermediate values within the range. Thus, it is predicted that intercalation in 2D-COFs can yield spintronic half-metal behavior. Furthermore, it is possible to achieve a wide range of bandgaps, depending on the concentration and position of intercalants, opening their application in next-generation spin-based electronics. As an example, in Figure we plot the structure and spin-polarized electronic properties of 2D-COF-Ni-05. This material has conducting spin up states, while the spin down channel shows a semiconducting 1.32 eV bandgap. We observe that the spin up conducting states mainly come from carbon contributions. The spin down semiconducting channel, mostly presents carbon contributions at the CBM, and the VBM is primarily comprised of nickel and nitrogen orbitals. The interactions between COF d-orbitals and TM p-orbitals again become essential to provide states that result in enhanced electronic/magnetic properties, in this case, half metal behavior. Spin-up and spin-down band edges are plotted separately in Figure , allowing us to easily observe which materials are potential candidates for other spintronic applications. Within the semiconducting 2D COFs that were analyzed, we find some materials with off-shifted spin-up and spin-down band edges, i.e., spin-up and spin-down VBM and CBM have different relative positions. Within our intercalated structures, we find five materials that clearly present half-semiconducting character: Co-04a, Co-04b, Cr-02, Mn-04a, and V-01a. These materials present a wide bandgap in one of their spin channels and narrow bandgap in the other spin channel. Furthermore, half semiconductors have their VBM and CBM in the same spin channel, allowing to produce 100% polarized electrons through photon or thermal excitation. To exemplify this effect, in Figure we plot the band structure and DOS for Mn-04a. This material presents a direct narrow bandgap of 0.57 eV in its spin-down channel and an indirect wide spin-up bandgap of 2.1 eV in its spin-up channel, making spin-down electron transitions much more likely to occur not only due to their bandgap values but also their bandgap type (small direct bandgap vs wide indirect bandgap). Therefore, this material is an ideal candidate for the generation of 100% spin-down polarized electrons. Similar to our optoelectronic and half-metal materials, this spintronic behavior is heavily mediated by Mn 3d-orbitals, which are hybridized with carbon, boron, and oxygen 2p-orbitals and are important contributors to the DOS near the band edges. Figure also reveals that the band alignments for eleven of our materials have potential as bipolar magnetic semiconductors (BMS): Cu-02, Fe-01a, Fe-01b, Mn-01a, Mn-01b, Sc-02, Ti-04a, Ti-04b, V-02, V-04b and V-05. These spintronic semiconducting materials have their VBM and CBM fully polarized in the opposite spin direction, with their spin-up and spin-down channels off-shifted. In BMSs, it is possible to generate fully spin-polarized electrons by applying a gate voltage. Taking V-05 as an example (see Figure ), under zero gate voltage it presents semiconducting behavior. Further, at an appropriate negative gate voltage, the Fermi level is shifted down (in the vacuum scale), resulting in a conductive spin-up channel and semiconducting spin down-channel. Additionally, at an appropriate positive gate voltage, the Fermi level is shifted up, resulting in a conductive spin-down channel and semiconducting spin-up channel. Even though 2D-COF-V-05 presents appropriate BMS band edges, its density of states has large gaps within the band structure, making it difficult for electrons to travel throughout the material. To remedy this issue and increase the electronic states in the system, as proof of concept, we added another fully-intercalated V-05 2D COF layer. We present these results in Figure . In this plot, we observe a rearrangement of electronic states when adding a third COF layer and intercalants, where now a positive gate voltage would generate a conductive spin-up channel and a negative voltage would generate a conductive spin-down channel. Most importantly, the large gaps below the VBM and above the CBM are substantially reduced, which results in enhanced available electronic states within the material. This is an important result, as we see that spintronic behavior in 2D COFs can be fine tuned by the number of layers, which is an effect that has not been researched in the past for this family of compounds.