Herein, poly(N-(4-aminophenyl)methacrylamide)-carbon nano-onions [abbreviated as PAPMA-CNOs (f-CNOs)] integrated gallic acid cross-linked zein composite fibers (ZG/f-CNOs) were developed for the removal/recovery of phosphate from wastewater along with controlled drug delivery and intrinsic antibacterial characteristics. The composite fibers were produced by Forcespinning followed by a heat-pressure technique. The obtained ZG/f-CNOs composite fibers presented several favorable characteristics of nanoadsorbents and drug carriers. The composite fibers exhibited excellent adsorption capabilities for phosphate ions. The adsorption assessment demonstrated that composite fibers process highly selective sequestration of phosphate ions from polluted water, even in the presence of competing anions. The ZG/f-CNOs composite fibers presented a maximum phosphate adsorption capacity (q max ) of 2500 mg/ g at pH 7.0. This represents the most efficient phosphate adsorption system among all of the reported nanocomposites to date. The isotherm studies and adsorption kinetics of the adsorbent showed that the adsorption experiments followed the pseudo-second-order and Langmuir isotherm model (R 2 = 0.9999). After 13 adsorption/desorption cycles, the adsorbent could still maintain its adsorption efficiency of 96−98% at pH 7.0 while maintaining stability under thermal and chemical conditions. The results mark significant progress in the design of composite fibers for removing phosphates from wastewater, potentially aiding in alleviating eutrophication effects. Owing to the f-CNOs incorporation, ZG/f-CNOs composite fibers exhibited controlled drug delivery. An antibiotic azithromycin drugencapsulated composite fibers presented a pH-mediated drug release in a controlled manner over 18 days. Furthermore, the composite fibers displayed excellent antibacterial efficiency against Gram-positive and Gram-negative bacteria without causing resistance. In addition, zein composite fibers showed augmented mechanical properties due to the presence of f-CNOs within the zein matrix. Nonetheless, the robust zein composite fibers with inherent stimuli-responsive drug delivery, antibacterial properties, and phosphate adsorption properties can be considered promising multifunctional composites for biomedical applications and environmental remediation.