Shape-persistent macrocycles and 3D nanocages have been prepared in one-pot under MeCN-promoted dynamic covalent bond conditions starting from silane catecholates, whose structures were confirmed by X-ray crystallography. Cation-exchange reactions of macrocycles and nanocages were performed along with the encapsulation of ammonium ions within the cavity of an anionic macrocycle and a tetrahedral nanocage.