The magnetooptical (MO) response of Ru/Py/Ta thin film stacks with 4, 8, and 17 nm thick Ni81Fe19 permalloy (Py) films on a SiO2/Si and a ZnO substrate was measured by vector magnetooptical generalized ellipsometry. The MO response from VMOGE was modelled using a 4 × 4 Mueller matrix algorithm. The wavelength-dependent, substrate-independent and thickness-independent complex MO coupling constant (
Q
) of Py in the Ru/Py/Ta thin film stacks was extracted by fitting Mueller matrix difference spectra in the spectral range from 300 nm to 1000 nm. Although the composition-dependent saturation magnetization of Ni
x
Fe1−x
alloys (x = 0.0…1.0), e.g. of Ni81Fe19, is predictable from the two saturation magnetization end points, the MO coupling constant of Ni
x
Fe1−x
is not predictable from the two
Q
end points. However, in a small alloy range (0.0 < x < 0.2 and 0.8 < x < 1.0) the composition-dependent
Q
of Ni
x
Fe1−x
can be interpolated from a sufficiently high number of analyzed Ni
x
Fe1−x
alloys. The available complex MO coupling constants of six different Ni
x
Fe1−x
(x = 1.0 to 0.0) alloys were used to interpolate MO response of binary Ni
x
Fe1−x
alloys in the range from x = 0.0 to x = 1.0.