We report the solution-phase formation of ordered lamellar nanocrystal (NC) arrays. These semiconductor lamellae exhibit structural integrity and temporal stability, without recourse to chemical crosslinking. They are many micrometers in diameter yet only two or three nanocrystal layers in thickness. We show that these structures can integrate a cargo of water-soluble ions, molecules, metal nanoparticles, or biomolecules. Encapsulation of gold nanoparticles is found to cause photoluminescence enhancement of the host CdSe nanocrystals. These easily prepared nanocrystal "envelopes" promise properties modulated through the integration of a vast array of water-soluble species. Our approach marks a step toward ordered, compartmentalized, NC-based complexes with controlled architectures.