Comparative DFT calculations for eleven all-silica zeolites showed a significant variation in the CBZ adsorption energies, demonstrating the usefulness of considering different topologies when trying to develop optimized zeolite adsorbents for selective CBZ removal. IFR, AFI, and CFI were identified as frameworks having the highest affinity, and the all-silica zeolites ITQ-4, SSZ-24, and CIT-5 can hence be proposed as target materials for future experimental studies.