We report the observation of strong third-harmonic generation from a macroscopic array of aligned ultralong single-wall carbon nanotubes (SWCNTs)with intensemidinfrared radiation. Through power-dependent experiments, we determined the absolute value of the third-order nonlinear optical susceptibility !(3) of our SWCNT film to be 5.53 × 10−12 esu, three orders of magnitude larger than that of the fused silica reference we used. Taking account of the filling factor of 8.75% for our SWCNT film, we estimate a !(3) of 6.32 × 10−11 esu for a fully dense film. Furthermore, through polarization-dependent experiments, we extracted all the nonzero elements of the !(3) tensor, determining the magnitude of the weaker tensor elements to be #1/6 of that of the dominant !(3) zzzz component.