Chiral metal-organic frameworks (CMOFs) exhibit significant potential for circularly polarized luminescence (CPL) due to their effective cooperation of chirality and luminescence. Herein, we utilize circularly polarized fluorescence energy transfer (CPF-ET) as a guiding principle to engineer CPL-active CMOFs through ligand functionalization. Three pairs of enantiomeric CMOFs were synthesized from optically pure chiral benzimidazole-derived ligands and substituted phenyl dicarboxylic acids. The resulting Cd-based CMOFs feature qzd topology and exhibit tunable CPL behaviors dependent on the substituents. Notably, while S/R-1 shows a negligible CPL response, its isomorphic analogue S/R-1-NH2 achieves a significantly enhanced |glum| of 5.3 × 10-3. The substantial impact of ligand functionalization on CPL performance, demonstrated across the series, highlights its critical role and provides a rational design strategy for advanced chiral photonic materials based on the CPF-ET mechanism.