Solid-state deuterium NMR spectroscopy is used to study the dynamics of organic molecules occluded in the as-synthesized high-silica tectosilicate nonasil. The nonasil samples are synthesized using trimethylalkylammonium structure-directing agents to determine the role of electrostatic interactions. Size effects are quantified by performing H-2 NMR spin-lattice (T-1) relaxation experiments, and the mobility of the substituent alkyl groups is studied using H-2 MAS NMR. The charge-compensating defect sites are characterized using Si-29 and H-1 NMR. The motion of the trimethylammonium group of the structure-directing agent is a composite motion of methyl group rotations and rotation about the nitrogen C-3 axis in all samples down to 190 K. The H-2 T-1 and H-2 MAS NMR results illustrate the steric confinement the nonasil cage exerts on the larger (C-n greater than or equal to C-5) subsequent alkyl groups. Isotropic motion is not observed for any of the structure-directing agents at 370 K, indicating strong organic-inorganic interactions. This is in sharp contrast to nonasil samples made with electrically neutral amines where rapid isotropic reorientation is observed at room temperature. These results have interesting implications in zeolite synthesis. For aluminosilicates synthesized with charged structure-directing agents, similar organic-inorganic interactions may allow for aluminum preferentially occupying specific framework sites. This could lead to tailoring the distribution of catalytic sites in zeolites based on the charge distribution of the structure-directing agent.