1 of 7) 1600575 direct laser writing, as opposed to longer pulses, is that they can rapidly deposit energy in solids with high precision. The light is absorbed and the optical excitation ends before the surrounding lattice is perturbed, which results in highly localized nanostructuring without collateral material damage. [19,20] First observation of laser-induced periodic surface structures dates back to the 1960s, when Birnbaum reported ripple formation on the surface of semiconductors. [21] Since then, this phenomenon was observed on virtually any type of media including metal, semiconductor, dielectric solids, and thin films. [22][23][24][25][26][27][28][29] Processing conditions occurred to be broad with wavelengths ranging from the mid-infrared to visible spectrum and from continuous wave operation to femtosecond laser systems. A vast number of applications, including coloration, [30] control of surface chemical and mechanical properties, [31,32] have been proposed.More than a decade ago, Bricchi and Kazansky demonstrated that femtosecond laser pulses focused inside silica glass can lead to self-assembled nanogratings, which exhibit birefringence comparable to quartz crystals. [33] Later, the tailored surface nanogratings were introduced showing the threefold birefringence increase. [34] Thus, a functional birefringent layer should be at least several tens of micrometers thick. For most applications such a thickness is appropriate. However, this limits the design and integration of miniaturized elements.To realize the laser-induced nanogratings as functional metasurfaces, the intermediate case between volume and surface periodic structuring has to be implemented when the modification of high-index thin films along its depth would significantly enhance the resulting anisotropy. Here we demonstrate that the interaction of femtosecond laser pulses with hydrogenated amorphous silicon (a-Si:H) thin films induces self-assembled periodic lamellae structures oriented perpendicular to the incident beam polarization. These films with the induced subwavelength modulation of refractive index behave as a uniaxial birefringent material with the slow axis oriented parallel to the imprinted nanogratings. Thus, the form birefringence of two orders of magnitude higher than in silica glass can be achieved. [18,[33][34][35] As a result, large retardation is realized within hundreds of times thinner layers (Figure 1a) that can be deposited on various substrates with different textures.We leverage the realization of laser-induced periodic thinfilm structures as a highly birefringent metasurface to design controllable and high precision GPOEs. Here we report on demonstration of various geometric phase designs including arrays of polarization microconverters and microlenses, polarization gratings (PGs) and computer-generated holograms with phase gradients reaching up to ≈1 rad µm −1 .In order to identify the maximum birefringence of the laser-induced periodic thin-film structures, 80 µm long lines