1. Permethylation at the 2 and 6 positions leads to up to 4-fold stronger binding of some of these guest molecules. 2. TDZ is consistently the strongest binder, with a dissociation constant as low as 18 µM in the case of H26DM-βCD, surpassing that of rimantidine with native βCD. 3. Chlorpromazine binds consistently more strongly than promazine, with a Kd nearly 5-fold lower in the case of H6M-βCD. 4. The enthalpy of binding is strongly favorable in all cases, and the thermodynamic data fall on a classic entropy-enthalpy compensation line. 5. 2D NMR studies show that all guests position at least one aromatic proton at the secondary face of the CD in all cases, and most also have NOEs to H5, indicating deep penetration of the binding site. 6. TDZ and TFP have additional NOEs between their cationic side-chains and protons at the primary face.