Fe3+ is one of the crucial metal ions in biological systems, and its excess or deficiency in the body can trigger various diseases, posing a serious threat to human health. Moreover, improper handling or disposal of Fe3+ can lead to water pollution, thereby harming the environment. Therefore, the development of highly selective and sensitive Fe3+ detection probes is particularly urgent. In this paper, a dual-mode sensor based on sol-gel and fluorescence signal responses was developed for the visual detection of Fe3+. The visual sensing method based on the simultaneous response of Fe3+-triggered dual signals can minimize the interference from false-positive signals and enhance detection accuracy. The dual-mode sensor, denoted as PAA@CDs, was constructed by incorporating high-brightness (high fluorescence emission intensity) green-yellow carbon dots (CDs) into poly(acrylic acid) (PAA), which possesses a large number of carboxyl functional groups. Based on the interaction of Fe3+ with the surface functional groups of CDs, nonfluorescent complexes are formed, leading to nonradiative electron transfer, which induces fluorescence quenching and produces a fluorescence signal visible to the naked eye. Additionally, the interaction of Fe3+ with the carboxyl groups of PAA triggers the cross-linking of PAA, causing a sol-gel phase change signal. Consequently, the PAA@CDs exhibit a dual-response signal in Fe3+ detection. Based on the fluorescence method, the linear detection range of PAA@CDs for Fe3+ is 0.05-2.60 mM with a limit of detection (LOD) of 5.14 μM. Meanwhile, using the sol-gel method, the linear detection range is 0.02-2.20 mM, and the LOD is 42.5 μM. Furthermore, the PAA@CDs probes can be successfully applied to the detection of Fe3+ in real water samples, demonstrating their potential value in the analysis of real samples containing multiple ions.