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Herein, we report the emergence of multicolor photoluminescence in a mixed-valence manganite nanoparticle La_0.67Sr_0.33MnO₃ (LSMO NP) achieved through electronic structural modification of the nanoparticles upon functionalization with a biocompatible organic ligand, sodium tartrate. From UV–vis absorption, X-ray photoelectron spectroscopy (XPS), time-resolved photoluminescence study, and Raman spectroscopic measurements, it is revealed that ligand-to-metal charge transfer transitions from highest occupied molecular orbital (HOMO, centered in tartrate ligand) to lowest unoccupied molecular orbital (LUMO, centered in Mn^3+/4+ of the NPs), and d–d transitions involving Jahn–Teller sensitive Mn³⁺ ions in the NPs plays the central role behind the origin of multiple photoluminescence from the ligand functionalized LSMO NPs.