Color‐tunable luminescent materials based on α, ω‐diethyl malonate terminated polydimethylsiloxane (EP) and lanthanide ions are synthesized. The EP is synthesized from α, ω‐hydride terminated polysiloxane (HP) and diethyl allyl malonate via hydrosilylation reaction. The FT‐IR spectra, 1H NMR, 13C NMR, and GPC are used to characterize the structures of HP and EP. The obtained materials, which were synthesized by incorporating Eu3+ (or Tb3+) ions into EP, exhibit excellent narrow‐width red (or green) emissions. Moreover, when integrating heterometallic Eu3+/Tb3+ ions into EP, the luminescence spectra of the complexes are composed of green and red emission. Color‐tunable luminescent materials are obtained by tuning the proportions of Eu3+ and Tb3+ ions. magnified image

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