This is the first report on the synthesis of a new functional nanocomposite gel containing amidoxime functionalized multiwall carbon nanotube (AO-MWNT-FNC GEL). The surface morphology of AO-MWNT-FNC GEL was investigated by field emission scanning electron microscopy. The modification of gel with amidoxine groups was confirmed by Fourier transform infra red spectroscopy. The AO-MWNT-FNC GEL provides effective binding with uranium ions as was ascertained by X-ray photoelectron spectroscopy. The AO-MWNT-FNC GEL was utilized as the new adsorbent for the recovery of uranium ions from aqueous solution. UV-visible spectroscopy was used to monitor the adsorption capacity of the AO-MWNT-FNC GEL toward uranium ions. The influence of initial uranium ion concentration and solution pH on the adsorption capacity of the AO-MWNT-FNC GEL were studied in batch experiments. The new FNC-GEL designed in this study is distinguished by higher adsorption capacity for uranium ions due to the synergistic contributions from high surface area of MWNT and the functional AO groups in FNC-GEL and exhibits potential for efficient recovery of uranium ions.