A simple approach for the functionalization of cylindrically shaped zeolite L crystals with iron oxide magnetic nanoparticles is reported. These functionalized zeolites can be aligned very easily by applying a magnetic field in solution, on different substrates, and in a polymeric matrix. The aligned zeolite loaded with fluorescent dyes are anisotropic in both absorption and fluorescence owing to the linear arrangement of the channels and the restricted rotation of the molecules inside the channels. These findings can be applied on polymeric matrices, such as poly[3-3'(vinylcarbazole)].The manipulation and orientation of nano-/micro-objects by using an external stimulus is of great interest to organize these entities in a hierarchical manner to obtain cooperative or bulk effects. In particular, light and magnetism have been applied to nanoparticles, beads, rods, and nano-/mesoporous materials [1][2][3][4][5] as a stimulus to assembly them in solution and on solid surfaces.The idea of combining porosity and magnetism opens up the opportunity for many new applications, for example, the immobilization of proteins, [6] delivery vehicles, [7] or other bioapplications. [8,9] Furthermore, the analytical use of magnetic separation is widely employed in biotechnology, [10] and in biomedical areas, such as drug delivery/release, [11a] DNA probes, [11b] or switches for biocatalytic applications that rely on magnetic triggering. [8] The organization of porous materials in polymers or surfaces and the use of loaded molecules to impart new properties to the aligned systems have been less explored. Among amorphous and crystalline porous materials, zeolites enable a high control of the size, shape, and loading. This permits restriction of the porosity to unidimensional channels that lead to a linear arrangement of entrapped molecules, which result in new optical, electrical, and magnetic properties. [12] Zeolite L is an aluminosilicate with the nominal composition [K 9 (Al 9 Si 27 O 72 )·x H 2 O], which features a hexagonal framework that contains a unidimensional channel system with a pore opening of 7.1 . The presence of solvent molecules in the channels of the crystals and cations, which compensate for the negatively charged framework, provides the opportunity to exchange ions or molecules with an appropriate size. Zeolite L is a catalyst for a variety of reactions, such as hydrocracking or selective para-chlorination. [13,14] Along with their transparency in the visible spectral range, zeolite L permit the study of the photophysical properties of inserted organic dye molecules. [15][16][17][18][19] The leakage of the entrapped molecules can be easily prevented by applying a silica shell to the crystals. [20] Zeolite L has emerged as an appropriate host material for building artificial antenna systems, [21, 22] (unidirectional) energytransfer materials, [21,23] and for the self-assembly of fluorescent supramolecular systems [24][25][26] and patterns. [27] Also, it has been employed for imaging purposes [28] and as a bioco...