NiCo2S4 is a technologically important electrode material that has recently achieved remarkable performance in pseudocapacitor, catalysis, and dye-synthesized solar cell applications.1 5 Essentially, all reports on this material have presumed it to be semiconducting, like many of the chalcogenides, with a reported band gap in the range of 1.2-1.7 eV.6,7 In this report, we have conducted detailed experimental and theoretical studies, most of which done for the first time, which overwhelmingly show that NiCo2S4 is in fact a metal. We have also calculated the Raman spectrum of this material and experimentally verified it for the first time, hence clarifying inconsistent Raman spectra reports. Some of the key results that support our conclusions include: (1) the measured carrier density in NiCo2S4 is 3.18 × 1022 cm-3, (2) NiCo2S4 has a room temperature resistivity of around 103 cm which increases with temperature, (3) NiCo2S4 exhibits a quadratic dependence of the magnetoresistance on magnetic field, (4) thermopower measurements show an extremely low Seebeck coefficient of 5 V K-1, (5) first-principles calculations confirm that NiCo2S4 is a metal. These results suggest that it is time to rethink the presumed semiconducting nature of this promising material. They also suggest that the metallic conductivity is another reason (besides the known significant redox activity) behind the excellent performance reported for this material. © 2015 American Chemical Society.