The Mueller matrix elements m_ij representing the polarization response from a nanostructured materialis determined by the constituent materials optical properties and the superstructure. Here, we investigate how chiral structures in form of helicoidally stacked uniaxial layers determine m_ij as a functionof polarization state, wavelength, incidence angle and azimuthal angle of the incoming light. The studied parameters include the layer materials ordinary/extraordinary optical properties, Euler angle values, and layer thickness as well as the thickness and pitch of the helicoidal superstructure. Sub- and superstructure inhomogeneity is also introduced. From the Fresnel-based calculations, m_ij aswell as the degree of polarization, ellipticity and azimuth of the polarization ellipse are obtained and presented as contour and trace plots to give a complete view of the polarization behavior. The results from the calculations are compared with Mueller matrix spectroscopic ellipsometry measurements of both natural and synthesized helicoidal structures. The measurements were performed with a dualrotating compensator system (RC2, J.A. Woollam Co., Inc.) for wavelengths in the range from 245 to 1000 nm and incident angles from 20 to 75°. For some measurements the azimuthal angle of the incident light was varied. The investigated natural chiral structures were exoskeletons from several beetles in the scarab subfamilies Cetoniinae and Rutelinae. As predicted from the calculations it isobserved that the reflection from these beetles can have a high degree of polarization and high ellipticity (near-circular polarization). Both left- and right-polarization was observed. The synthesized structures are helicoidal nanorods of Al_1−xIn_xN grown on sapphire substrates with metal-nitride seedlayers using UHV magnetron sputtering. Due to an internal composition gradient (a variation of x) in the crystalline structure, the nanorods will tilt away from the substrate normal. Helicoidal structures can thus be obtained by rotating the substrate around its normal during deposition. Samples with different pitch and layer thickness with right-handed as well as left-handed chirality were grown. Also for these structures both left and right near-circular polarized light is observed. By combining calculations, ellipsometry measurements and scanning electron microscopy characterization we get agood input to build layered models of the natural and synthetic samples. After regression fitting agood agreement between calculated and measured optical data were obtained.