The ongoing search for new photorefractive materials offering a high photosensitive flexibility is triggered by the limited tuning ability of conventional photorefractive materials, such as electro-optic crystals, photopolymers, or liquid crystals. One of the latest discovered photorefractive materials is Na 2 [Fe(CN) 5 NO] · 2H 2 O, in which metastable linkage isomers of the nitrosyl group can be generated by light irradiation resulting in huge changes of the refractive index up to Dn ∼ 10 -2 .Here we show that this type of photorefraction is a general property arising from the generation of linkage isomers and can thus be found in many compounds containing [ML 5 NO] m± complexes, where M is a transition metal, L a ligand, and m the formal charge of the anion/cation. The benefit of this generality is reflected in the tailoring properties of the photorefractive response such as the spectral sensitivity simply by selecting different representatives of the [ML 5 NO] m± compounds.Conventional photorefractive materials, [1] where the lightinduced modulation of the refractive index is caused by the linear electro-optic effect (Pockels effect), are widely applied in nonlinear optics.[2] They feature reversible photorefractivity without chemical processing allowing for dynamical holography, [3] and the kinetics of hologram formation is described by the well-known Kiev equations. [4] In recent years a second class of reversible photorefractive media for dynamical holography has been established, the unconventional photorefractive materials. Here an optical bistability is at the origin of photorefraction and the kinetics show a characteristic transient behavior.[5] The unique properties of this class were com-