Carboxylated PIM-1 fibers were prepared by one-step hydrolysis of PIM-1 fibers using sodium hydroxide solution. The chemical structure and morphology of the hydrolyzed PIM-1 fibers were characterized. The adsorption behaviors of the hydrolyzed PIM-1 fibers towards different organic dyes and heavy metal ions in an aqueous solution were investigated. The results showed that the hydrolyzed PIM-1 fibers could effectively adsorb methylene blue (MB), safranin O (SO), and methylene violet (MV), but barely adsorb methyl orange (MO), indicating a selective adsorption property. Isotherm studies revealed that the Freundlich model was more suitable for describing the adsorption behavior of the hydrolyzed PIM-1 fibers than the Langmuir model. The adsorption mechani** was investigated by UV–vis absorbance spectra and solution pH effect. It was concluded that the adsorption process was based on the host–guest interactions between the hydrolyzed PIM-1 fibers and the dyes. In addition, the hydrolyzed PIM-1 fibers exhibited an improved adsorption capacity for heavy metal ions (41.2 mg/g for Pb2+, 16.9 mg/g for Cu2+, respectively) than the pristine PIM-1 fibers. Based on our results, the hydrolyzed PIM-1 fibers, as an easily prepared adsorbent material, show potential application for the selective removal of various organic dyes and heavy metal ions in wastewater treatment.