This study proposes a novel strategy to enhance the performance of white light-emitting diodes (WLEDs) by integrating graphitic carbon nitride (g-C3N4) as an independent blue emitter into Tb3+/Eu3+-doped lanthanide metal–organic frameworks (Ln-MOFs). Traditional Ln-MOF-based WLEDs suffer from low luminous efficiency due to the Antenna Effect, which compromises energy transfer between ligands and lanthanide ions. By incorporating g-C3N4 with high-concentration Tb3+/Eu3+-doped Ln-MOFs, the optimized composite material, g-C3N4@Tb0.95Eu0.05-MOF, demonstrated remarkable improvements in photoluminescence properties. Compared to conventional Gd0.978Tb0.02Eu0.002-MOF, the composite achieved a luminous flux of 1.24 lm, luminous efficacy of 1.66 lm/W, and color rendering index (CRI) of 91.6, representing 10.34-fold, 9.23-fold, and 9.0 enhancements, respectively. Mechanistic studies revealed no energy transfer between g-C3N4 and Ln3+ ions, enabling stable blue emission from g-C3N4 while high-concentration Tb3+ and Eu3+ ions enhanced green and red emissions. This work provides a promising approach for designing high-performance WLEDs.