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A single-wall carbon nanotubes (SWNT) film coated glassy carbon electrode (GCE) was fabricated for the direct determination of 4-nitrophenol (4-NP). The electrochemical behaviors of 4-NP at the SWNT-film coated GCE were examined. In 0.1 M phosphate buffer with a pH of 5.0, 4-NP yields a very sensitive and well-defined reduction peak at the SWNT-modified GCE. It is found that the SWNT film exhibits obvious electrocatalytic activity towards the reduction of 4-NP since it not only increases the reduction peak current but also lowers the reduction overpotential. Based on this, an electrochemical method was proposed for the direct determination of 4-NP. The reduction peak current varies linearly with the concentration of 4-NP ranging from 1 × 10−8 to 5 × 10−6 M, and the detection limit is 2.5 × 10−9 M after 3 min of open-circuit accumulation. The relative standard deviation at 2 × 10−7 M 4-NP was about 6% (n = 10), suggesting excellent reproducibility. This new method was successfully employed to determine 4-NP in several lake water samples.