Due to its extreme kinetic inertness, trivalent chromium, Cr(III), has been rarely combined with labile trivalent lanthanides, Ln(III), to give discrete self-assembled (supra)molecular polynuclear complexes. However, the plethora of accessible metal-centered excited states possessing variable lifetimes and emissive properties, combined with the design of efficient intramolecular Cr(III)↔Ln(III) energy transferprocesses open attractive perspectives for programming directional light-conversion within these heterometallic molecules. Efforts made to address this exciting challenge for both light-sensitization and light-upconversion are discussed in this article.