Two-photon absorption excited intramolecular energy transfer and light-harvesting effects are demonstrated in three novel dendritic systems. These systems contain both an antenna structure that can effectively absorb two-photon energy at approximately 800 nm and emit fluorescence at approximately 515 nm and a core moiety that can absorb one-photon energy at approximately 520 nm and emit at approximately 590 nm. Covalently combining the core and antenna functionalities intrinsically changes the optical behavior of the component pieces. The two-photon energy absorbed by the antenna structure is resonantly transferred to the core, where the core's emission intensity is enhanced by 8, 20, and 34 times for the three dendritic systems.