Gelest, Inc., Morrisville, PA) were used as obtained. House-deionized water was purified using a Millipore Milli-Q-filtering system containing one carbon and two ion-exchange stages. Experimental methods that were used to (i) synthesize 5,11,17,23,29,35hexakis[(N,N,N-trimethylamonium)-N-methyl-37,38,39,40,41,42-hexakis-nhexadecyloxy-calix[6]arene chloride (i.e., Calix), (ii) deposit Langmuir-Blodgett (LB) bilayers of PAA-crosslinked Calix, 1 and 2 onto poly[1-(trimethylsilyl)-1-propyne] (PTMSP) supports or silicon wafers (silylated with n-octadecyltrichlorosilane, OTS), (iii) quantify gas permeabilities, and (iv) measure film thicknesses by ellipsometry were similar to those that have previously been described. [1][2][3] Ellipsometry measurements were made using VASE ellipsometer (J.A. Woollam Co., Inc., Lincoln, NE), equipped with variable wavelength ( from 250-1700nm) and angle of incidence (15º-90º) system, a λ of 632.8nm and an incidence angle of 70º were chosen for measurements. The refractive indices that were used to estimate the thickness of the OTS and the LB bilayers were both 1.46. All AFM measurements were made using a tapping mode atomic force microscopy