DFT calculations in Table were performed using the def2-ma-SVP basis set and include counterpoise correction. This procedure affords negligible basis-set convergence errors in supramolecular DFT calculations, and tests on (half-COF1) 2 in Table demonstrate that counterpoise-corrected DFT/def2-ma-SVP interaction energies are converged to within 1 kcal/mol of DFT/def2-TZVPD results. Basis set effects are somewhat larger (∼ 3 kcal/mol) at the XSAPT+MBD level (Table ), although the energetic ordering of various structures is conserved upon enlarging the basis set from def2-ma-SVP to def2-ma-TZVP. Since total interaction energies exceed 40 kcal/mol even for (half-COF1) 2 , we regard this as semiquantitative. The largest discrepancy between the two basis sets occurs between the (0,0) and (1 Å,1 Å) structures, where the exchange-repulsion energy is largest. This is consistent with the observation that E exch exhibits the slowest convergence of the XSAPT+MBD energy components. The hex-COF1 monomer has twice as many atoms as the original COF-1 monomer unit and the 3COF1 monomer has almost three times as many atoms, and interaction energies for the dimers scale accordingly. The eclipsed-cofacial or (0,0) structure is consistently higher in energy as compared to the slip-stacked structure with ∆x = 1 Å = ∆y, which is lowest in energy at each level of theory that is examined. This consistency across various model systems suggests that the original (COF1) 2 model affords a reasonable description of short-range interactions in the real material.