Resumen: We report the deposition of monolayers and multilayers of {Cr10(OMe)20(O2CCMe3)10} wheels, hereafter {Cr10}, onto Au(111) and Cu(111) single‐crystal substrates, and their characterization combining scanning tunneling microscopy, X‐ray photoelectron spectroscopy, X‐ray absorption spectroscopy, X‐ray natural linear dichroism, and X‐ray magnetic circular dichroism (XMCD). {Cr10} in bulk shows axial magnetic anisotropy and a cluster total spin S = 9 ground state, stemming from an interaction scheme of two semi‐crowns containing four Cr3+ ions interacting ferromagnetically, separated by two Cr3+ antiferromagnetically coupled. The one‐monolayer (1ML) samples of {Cr10} sublimated on Ag(111) and Cu(111) show slightly different applied magnetic field dependence of XMCD signal. The field‐dependence of the magnetization evolves from a lower curve for the 1ML {Cr10} samples to a curve resembling the bulk one as the number of layers is increased, as shown in a 14ML sample. Monte Carlo simulations allow rationalizing the magnetization curves of the 1ML samples in terms of a reduction of the cluster ground‐state total spin, S = 3 or S = 6, as a consequence of variations in the intra‐wheel coupling interactions induced by the on‐surface deposition. The sensitivity of the magnetic configuration of {Cr10} to minor distortions of the intramolecular conformation might be exploited to control magnetism by external stimuli for applications. Idioma: Inglés DOI: 10.1002/admi.202300146 Año: 2023 Publicado en: Advanced Materials Interfaces 10, 20 (2023), 2300146 [15 pp.] ISSN: 2196-7350 Factor impacto JCR: 4.3 (2023) Categ. JCR: CHEMISTRY, MULTIDISCIPLINARY rank: 71 / 230 = 0.309 (2023) - Q2 - T1 Categ. JCR: MATERIALS SCIENCE, MULTIDISCIPLINARY rank: 151 / 438 = 0.345 (2023) - Q2 - T2 Factor impacto CITESCORE: 8.4 - Mechanics of Materials (Q1) - Mechanical Engineering (Q1)