Enabling the use of rationally designed thin films in technological devices is a recognized goal in materials science. However, constructing such thin films using highly ordered supramolecular architectures with well-controlled size and growth direction has remained an elusive target. Here, we introduce a layer-by-layer protocol to grow hybrid thin films of molecule-based magnetic conductors comprising arachidic acid and donor bis(ethylenedioxy) tetrathiafulvalene (BEDO-TTF) as the organic component and Cu/Gd complexes as the inorganic component. The construction of layered hybrid thin films was achieved at ambient conditions by employing the Langmuir-Blodgett method, which provides good control over film thickness and packing of molecules in the monolayer. As demonstrated by X-ray diffraction, these films are crystalline with distinct organic and inorganic sublattices, where the BEDO-TTF molecular layer is interfaced with the inorganic layer. Due to the flexibility of the Langmuir-Blodgett deposition technique, this result indicates a route toward the preparation of well-ordered films with various functionalities, determined by the choice of the inorganic compound that is combined with the p-unit of BEDO-TFF. Moreover, the ability to deposit films on a variety of substrates establishes the potential for lower-cost device fabrication on inexpensive substrates.