The lanthanide fluoride clusters (py)₂₄Ln₂₈F₆₈(SePh)₁₆ (Ln = Nd, Pr) have been isolated and low temperature x-ray diffraction shows that they are comprised of a nearly spherical core of 28 Ln ions bridged by 68 µ3 and µ4 tetrahedral fluorides capped with doubly and triply bridging selenolates and terminal pyridines. These molecules offer new insight into the rational design of increasingly larger, optically important molecules with tailored photo emission properties. The optical properties of the Nd cluster we studied by optical absorption, photoluminescence and time resolved spectroscopy. Population of the ⁴F_3/2 excited state with a Ti:sapphire laser pumping at 800 nm gave rise to intense radiative emission for the ⁴F_3/2 → ⁴I_13/2 and ⁴F_3/2 → ⁴I_11/2transitions, corresponding to NIR emissions at 1339 nm and 1076 nm, respectively. The quantum efficiency (QE) for the 1076 nm emission was calculated to be 41%, the highest reported value for any molecular Nd species. The radiative fluorescence lifetime was found to be 739 µs, which is very close to the reported 800 µs lifetime found for solid state LnF3. Preliminary spectroscopic data for the Pr, Ce, and Nd:Pr clusters will be discussed.