In this study, the anticorrosion properties of a waterborne polyurethane dispersion (WPU) containing polyaniline (PAni) were investigated and discussed considering the electrical percolation threshold (EPT) of this mixture. For that, easily dispersible poly(styrene sulfonic acid)-doped PAni (PAni:PSS) was incorporated into an anionic WPU at contents ranging from 1 to 8 wt%. Free-standing films of PAni:PSS/WPU reached the EPT at 6 wt% (4.8 v.%) of PAni:PSS. The mixtures remained stable and without signs of PAni dedoping. Based on the electrical behavior curve, PAni:PSS/WPU coatings were prepared below (1, 2, 3 wt%), close to (5 wt%), at (6 wt%) and above the EPT (8 wt%). The coatings were applied on ground low-carbon steel panels and evaluated regarding their contact angle, adhesion, and anticorrosion performance in electrochemical tests. The coatings prepared below the EPT presented higher hydrophobicity, good wet adhesion, and higher open circuit potential (OCP) and impedance modulus in the low frequency range (|Z|10 mHz). The best overall performance was achieved at 3 wt% of PAni:PSS which presented OCP values in the range of 34 ± 11 mV for 144 h and initial |Z|10 mHz of 108 Ω.cm2. These coatings also presented a colorimetric feature of changing color as the corrosion progressed. Meanwhile, the coatings containing PAni:PSS quantities close, at and above the EPT, i.e., at 5, 6 and 8 wt% presented high porosity, poor wet adhesion, and intense blistering. They also presented OCP values in the region of active corrosion and impedance spectra typical of coatings with poor barrier properties. These results indicate that, the formation of conducting networks within the insulating matrix is not necessarily a condition that must be met for a coating containing PAni achieve an optimal anticorrosion performance.