The metalorganic frameworks (MOFs) with lanthanides ions offer great potential in the optical area because can provide properties of flexibility, low density, low-cost methods of synthesis, and insolubility in water, which give them an advantage over traditional phosphors. In this study, a thenoyltriflouroacetone ligand (TTA) with a Tb 3+ MOF was synthesized (Tb = 10 and 50% mol) and its structural and luminescent properties were analyzed. The metalorganic compound was generated in a simple one-pot reaction from terbium nitrate and 2-thenoyltrifluoroacetone precursors at room temperature. By means of FTIR, it was confirmed the presence of carbon groups, which made possible the terbium ion chelation, and also the Tb-O bonds vibration modes. 1 HNMR results confirm that the complex with 10% mol of Tb 3+ contains three coordinates molecules of TTA and two waters molecules. The powders exhibit rod-like morphology with size about 170 nm of diameter and a length about 2 μm; the rod-like nature of powders was confirmed by SEM and TEM analyses. By XRD it was concluded that at higher terbium concentration (TTA-50Tb sample) higher the crystallite size and crystallinity, in fact the TTA-10Tb sample shows a partial-amorphous nature. By photoluminescence analyses, the 5 D4→ 7 FJ (J = 3, 4, 5 and 6) emissions were recorded for both synthesized samples (λexc = 376 nm). Furthermore, it was observed that the emission intensity was enhanced in a factor of 3.5 for the TTA-50Tb. The energy transfer efficiency from TTA to Tb 3+ (antenna effect) was 0.984 for TTA-10Tb and 0.993 for TTA-50Tb. Decay time analyses indicate effective lifetime of 1.45 and 1.60 m s for the samples doped at 10 and 50%, respectively, indicating that the forbidden transition rules are stronger at higher crystallinity. The integrated intensities of the 5 D4 → 7 F5 (green at 541 nm) and 5 D4 → 7 F6 (blue at 486 nm) emissions and their intensity ratios IG/IB upon 376 nm excitation have been evaluated for TTA-10Tb andTTA-50Tb samples. The CIE1931 color of the MOFs excited at 376 nm attains a higher green color purity by increasing the terbium concentration. This is in concordance with the increased IG/IB ratio up for the TTA-10Tb and TTA-50Tb samples. Thus, the TTA-50Tb sample exhibits a green color purity of 67.94% with chromaticity coordinates (0.30, 0.57), being very close to those (0.29, 0.60) of European Broadcasting Union illuminant green. This interesting feature of the TTA-50Tb sample, together with an experimental branching ratio of 61.3% for the 5 D4 → 7 F5 green emission, highlights its capability as solid state green laser pumped by GaN (376 nm) LEDs.