Zeolites are crystalline aluminosilicates that are frequently used as catalysts to transform chemical feedstocks into more useful materials in a size- or shape-selective fashion; they are one of the earliest forms of nanotechnology. Zeolites can also be used, especially in the form of zeolite membranes (layers of zeolite on a support), to separate mixtures based on the size of the molecules. Recent advances have also created the possibility of using zeolites as alkaline catalysts, in addition to their traditional applications as acid catalysts and catalytic supports. Transport and catalysis in zeolites are greatly affected by physical and chemical defects. Such defects can be undesirable (in the case of zeolite membranes), or desirable (in the case of nitrogen-doped alkaline zeolites). Studying zeolites at the relevant length scales requires indirect experimental methods such as vapor adsorption or atomic-scale modeling such as electronic structure calculations. This dissertation explores both experimental and theoretical characterization of zeolites and zeolite membranes. Physical defects, important in membrane permeation, are studied using physical adsorption experiments and models of membrane transport. The results indicate that zeolite membranes can be modeled as a zeolite powder on top of a support—a “supported powder,” so to speak—for the purposes of adsorption. Mesoporosity that might be expected based on permeation and confocal microscopy measurements is not observed. Chemical defects—substitutions of nitrogen for oxygen—are studied using quantum mechanical models that predict spectroscopic properties. These models provide a method for simulating the 29Si NMR spectra of nitrogendefected zeolites. They also demonstrate that nitrogen substitutes into the zeolite framework (not just on the surface) under the proper reaction conditions. The results of these studies will be valuable to experimentalists and theorists alike in our efforts to understand the versatile and complicated materials that are zeolites.