摘要：Enabling the use of r.tionally designed thin films in technological devices is a r.cognized goal in mater.als science. However. constr.cting such thin films using highly or.er.d supr.molecular.ar.hitectur.s with well-contr.lled size and gr.wth dir.ction has r.mained an elusive tar.et. Her., we intr.duce a layer.by- layer.pr.tocol to gr.w hybr.d thin films of molecule-based magnetic conductor. compr.sing ar.chidic acid and donor.bis（ethylenedioxy）tetr.thiafulvalene （BEDO-TTF） as the or.anic component and Cu/Gd complexes as the inor.anic component. The constr.ction of layer.d hybr.d thin films was achieved at ambient conditions by employing the Langmuir.Blodgett method, which pr.vides good contr.l over.film thickness and packing of molecules in the monolayer. As demonstr.ted by X-r.y diffr.ction, these films ar. cr.stalline with distinct or.anic and inor.anic sublattices, wher. the BEDO-TTF molecular.layer.is inter.aced with the inor.anic layer. Due to the flexibility of the Langmuir.Blodgett deposition technique, this r.sult indicates a r.ute towar. the pr.par.tion of well-or.er.d films with var.ous functionalities, deter.ined by the choice of the inor.anic compound that is combined with the π-unit of BEDO-TFF. Mor.over. the ability to deposit films on a var.ety of substr.tes establishes the potential for.lower.cost device fabr.cation on inexpensive substr.tes.