The antibiotic Ciprofloxacin HCl (CPH) is a representative example of pharmaceutical contaminants of emerging concern that are frequently released in wastewater effluents and can cause hazardous health effects. In this work, we investigated the potential of utilizing porous polymeric membranes incorporating metal nanoparticles for removing CPH from water. In this regard, polylactic acid/polyurethane membranes were impregnated in situ with single, binary, and tertiary systems of nanoparticles of cobalt, copper, and nickel, among others. Membranes loaded with cobalt exhibited the best performance among all the examined membranes. They yielded removal efficiencies above 80% at an initial CPH concentration range of 10–50 ppm and pH 6.5, thus exceeding those of the bare membranes by about 1.3 times under the same conditions. As confirmed by Brunauer, Emmet, and Teller (BET) analysis, the incorporation of cobalt nanoparticles into the mesoporous membranes increased their surface area and pore volume by 5 and 10 times, respectively. Thermogravimetric analysis (TGA) showed that cobalt nanoparticles had no catalytic influence on the dissociation of the membrane polymeric chains. Fourier transform infrared (FTIR) and zeta potential measurements suggested that binding could possibly occur via physical interactions along with catalytic degradation.