Herein, we develop a novel method to synthesize lanthanide-functionalized carbon quantum dots via free-radical copolymerization using the methyl methacrylate (MMA) monomer as a functional monomer and introducing a lanthanide complex to obtain the dual-emission fluorescent composite material FCQDs-Ln(TFA) 3 (Ln = Eu, Tb; TFA: trifluoroacetylacetone). The obtained composites were fully characterized, and their structures were investigated by Fourier transform infrared spectroscopy (FTIR), 1 H NMR spectroscopy, X-ray photoelectron spectroscopy (XPS), and transmission electron microscopy (TEM). Subsequently, a series of white-light-emitting polymer composite films FCQDs-(Eu:Tb)(TFA) 3 /poly(methyl methacrylate) (PMMA) were designed and synthesized by adjusting the ratio of Eu(TFA) 3 /Tb(TFA) 3 under different wavelengths. More significantly, FCQDs-Tb(TFA) 3 was selected as a sensitive probe for sensing metal cations due to excellent photoluminescence properties, revealing a unique capability of FCQDs-Tb(TFA) 3 of detecting Fe(III) cations with high efficiency and selectivity. Furthermore, the sensing experiment results indicated that FCQDs-Tb(TFA) 3 is ideal as a fluorescent nanoprobe for Fe 3+ ion detection, and the lowest detection limit for Fe 3+ is 0.158 μM, which is superior to many other previous related research studies. This pioneering work provides a new idea and method for constructing a dual-emission ratio sensor based on carbon quantum dots and also extends the potential application in the biological and environmental fields.