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Single-molecule magnets (SMMs) hold promise for unmatched information storage density as well as applications in quantum computing and spintronics. To date, the most successful SMMs are organometallic lanthanide complexes. However, their surface immobilization, one of the requirements for device fabrication and commercial application, remains challenging due to sensitivity of magnetic properties to small changes in the electronic structure of the parent SMM. Thus, finding controlled approaches to SMM surface deposition is a timely challenge. In this contribution we apply the concept of isolobality to identify siloxides present at the surface of partially dehydroxylated silica as a suitable replacement for archetypal ligand architectures in organometallic SMMs. We demonstrate theoretically and experimentally that isolated siloxide anchorages not only enable successful immobilization, but also lead to two-orders-of-magnitude increase in magnetization relaxation times and provide magnetic site dilution.