Vector magneto-optical generalized ellipsometry on passivated ferromagnetic permalloy slanted columnar thin films is reported. The nanostructured thin film was grown by electron-beam glancing angle deposition and subsequently coated with a thin Al 2O 3 layer by atomic layer deposition. Magneto-optical generalized ellipsometry data have been acquired while an external magnetic field H with constant amplitude was rotated with respect to the sample (spatial hysteresis loops). The magneto-optical coupling parameters, which are proportional to the sample magnetization M, reveal intriguing anisotropic magnetic behavior of the slanted columnar thin film. Three-dimensional graphs of the magneto-optical coupling parameters with respect to spatial hysteresis loops shown here are representative for the sample magnetization.