Coordination-driven self-assembly delivers discrete, nanoscopic architectures that may preserve or enhance the physicochemical properties of their parent building blocks. Herein, we report the syntheses, characterization, and photophysical properties of two tetrahedral cages, [(Zn4L6)-L-II](PF6)(8) (C1) and [(Fe4L6)-L-II](OTf)(8) (C2), where L = Pt-II(PEt3)(2)(C equivalent to C-bpy)(2) (PEt3 = triethylphosphine; = 5-ethynyl-2,2'-bipyridine) and OTf = trifluoromethanesulfonate. C1 and C2 were assembled in isolated yields of 72% and 81% by treating 2 equiv of Zn(NO3)(2)center dot 6H(2)O or Fe(OTf)(2) with 3 equiv of L, respectively. Both cages were fully characterized by NMR, electrospray ionization mass spectrometry, and single-crystal X-ray diffraction (SCXRD). The local D-3 symmetry at each polypyridyl metal node raises the possibility of a number of isomeric cages; however, only the homochiral enantiomers (Delta Delta Delta Delta and Lambda Lambda Lambda Lambda) are formed based on H-1 NMR and SCXRD. Cl exhibits phosphorescence centered at 545 nm with a quantum yield of 10% in N-2-degassed acetonitrile at 25 degrees C. The quantum yield of C-2 is significantly lower due to a nonradiative relaxation from (MC)-M-5 (MC = metal-centered) states introduced by the Fe-II nodes.