We report on successful tests of holographically arranged grating-structures in nanoparticle-polymer compos-ites in the form of 100 microns thin free-standing films, i.e. without sample containers or covers that could cause unwanted absorption/incoherent scattering of very-cold neutrons. Despite their large diameter of 2 cm, the flexible materials are of high optical quality and yield mirror-like reflectivity of about 90% for neutrons of 4.1 nm wavelength