Figure S1 FT-IR spectra of (a) EuL, (b) EuL-bdc, and (c) Na2bdc in the KBr pellet. Figure S2 XPS (a) N1s (b) Eu3d, and (c) Tb3d bands of LnL (Ln=Eu or Tb, black), EuL-bdc (red), TbL-bdc (green) and [Eu0.5,Tb0.5](L)-bdc (blue). Binding energy was corrected at Au 4f level (84.0 eV) using gold powder. Figure S3 Top: FT-IR spectra of (a) EuL, (b) EuL-atpa, and (c) H2atpa in the KBr pellet. Bottom: (a) EuL, (b) EuL-htpa and (c) H2htpa in the KBr pellet. Figure S4 Top: (a) N 1s (b) Eu 3d, and (c) Tb 3d XPS bands of LnL (Ln=Eu or Tb; black line), EuL-atpa (red), TbL-atpa (green) and [Eu0.5,Tb0.5](L)-atpa (blue). Bottom: (d) N 1s (e) Eu 3d, and (f) Tb 3d XPS bands of LnL (Ln=Eu or Tb, black), EuL-htpa (red), TbL-htpa (green) and [Eu0.5,Tb0.5](L)-htpa (blue). Figure S5 Synchrotron X-ray powder diffraction patterns of (a-1) TbL-atpa, (a-2) [Eu0.5,Tb0.5](L)-atpa, (a-3) EuL-atpa, (b-1) TbL-htpa, (b-2) [Eu0.5,Tb0.5](L)-htpa, and (b-3) EuL-htpa. Figure S6 TGA (solid line) and DTA (dotted line) of (a) Eu(L)-bdc, (b) Eu(L)-atpa, (c) Eu(L)-htpa, and (d) EuL under nitrogen atmosphere at a heating rate of 10 °C min-1. Figure S7 Luminescence spectra of (a) EuL-bdc and (b) Eu-bdc after heat treatment (ex = 315 nm). Figure S8 Solid-state electronic absorption spectra of (a) EuL-bdc, (b) EuL-atpa, and (c) EuL-htpa, with that of EuL as a reference (dotted line). Figure S9 Phosphorescence spectra (ex = 315 nm) of (a) EuL-bdc, (b) EuL-atpa, and (c) EuL-htpa in the solid state, with that of EuL as a reference (dotted line). Figure S10 Excitation spectra monitored at 616 nm of EuL-bdc (solid line), EuL-atpa (dashed line), and EuL-atpa (dotted line). Figure S11 Schematic energy diagrams of [Eux,Tb1-x](L)-bdc. Figure S12 Emission decay curves of TbIII in (a) [Eux,Tb1-x](L)-atpa, and (b) [Eux,Tb1-x](L)-htpa at 77 K (x = 0 (green line), x = 0.5 (blue), and x = 0.9 (orange); ex = 315 nm, det = 544 nm). Table S1 Mixing ratio of Eu/Tb in [Eux,Tb1-x](L)-bdc determined by XPS Table S2 Mixing ratio of Eu/Tb in [Eux,Tb1-x](L)-atpa determined by XPS Table S3 Mixing ratio of Eu/Tb in [Eux,Tb1-x](L)-htpa determined by XPS Table S4 Luminescence lifetime τff of EuIII (and TbIII of [Eux,Tb1-x](L)-bdc at 77 K (λex = 315 nm, λdet = 615 nm for EuIII, λdet = 544 nm for TbIII)