A supramolecular host guest assembly composed of a cationic organic cavitand (host), neutral aromatic molecules (guests), and an anionic clay nanosheet has been prepared and demonstrated that in this arrangement efficient singlet singlet energy transfer could take place. The novelty of this system is the use of a cationic organic cavitand that enabled neutral organic molecules to be placed on an anionic saponite nanosheet. Efficient singlet singlet energy transfer between neutral pyrene and 2-acetylanthracene enclosed within a cationic organic cavitand (octa amine) arranged on a saponite nanosheet was demonstrated through steady-state and time-resolved emission studies. The high efficiency was realized from the suppression of aggregation, segregation, and self-fluorescence quenching. We believe that the studies presented here using a novel supramolecular assembly have expanded the types of molecules that could serve as candidates for efficient energy-transfer systems, such as in an artificial light-harvesting system.