Luminescent metal-organic frameworks (MOFs) (typically dye-encapsulated MOFs) are considered as one kind of interesting downconversion materials for white-light-emitting diodes (LEDs), but their quantum efficiency (QE) is not sufficient and thus needs to be significantly enhanced for practical applications. In this study, we successfully synthesized a series of Rh@bio-MOF-1 (Rh = rhodamine) with an internal QE as high as ∼79% via a solvothermal reaction followed by cation exchanges. The high efficiency of the Rh@bio-MOF-1 composites was attributable to the high intrinsic luminescent efficiency of the selected Rh dyes, the confinement effect in the bio-MOF-1 host, and the uniform particle morphology. The emission maximum could be continuously tuned from 550 to 610 nm by controlling the species and concentration of encapsulated dye molecules, showing great color tunability of the dye-encapsulated MOFs. The emission lifetime of ∼7 ns was 1 or 2 magnitude orders shorter than that of Ce- or Eu-doped inorganic phosphors, allowing for visible light communication (VLC). White LEDs, fabricated by using the synthesized Rh@bio-MOF-1 composite and inorganic phosphors of green (Ba,Sr)SiO:Eu and red CaAlSiN:Eu, exhibited a high color rendering index of 80-94, a luminous efficacy of 94-156 lm/W, and an excellent stability in color point against drive current. The Rh@bio-MOF-1 composites with tunable colors, short emission lifetime, and high QE are expected to be used for smart white LEDs with multifunctions of both lighting and VLC.