The present study aims to investigate the adsorption of synthesized poly(2-acrylamide-2-methylpropane sulfonic acid) (PAMPs) onto alumina nanoparticles and their application in the removal of ciprofloxacin (CFX) antibiotic from a water environment. The PAMPs were successfully synthesized and characterized by nuclear magnetic resonance and gel-permeation chromatography methods. The number- and weight-average molecular weights of PAMPs were 6.76 × 105 and 7.28 × 106 g/mol, respectively. The charge reversal of nanoalumina after PAMPs modification from positive to -37.5 mV was determined by ζ-potential measurement, while the appearance of C ═ O and N-H functional groups in PAMPs observed by Fourier-transform infrared spectroscopy confirmed them as the main indicators for adsorption of PAMPs onto a nanoalumina surface. The maximum adsorption capacity of PAMPs onto nanoalumina in 100 mg/L KCl was about 10 mg/g. The adsorption isotherms were fitted well by a two-step adsorption model. Application of PAMPs-modified nanoalumina (PAMNA) in CFX removal was also thoroughly studied. The optimum conditions for CFX removal using PAMNA were found to be pH 6, 10 mM NaCl, contact time 90 min, and adsorption dosage 5 mg/mL. The CFX adsorption isotherms and kinetics were in accordance with the two-step and pseudo-second-order models, respectively. The application for CFX removal in actual hospital wastewater was greater than 80%. The results of this study demonstrate that PAMNA is a new and promising material for antibiotic removal from wastewater.