Abstract: When molecules of a phenalenyl derivative, which has no net spin, are deposited on a ferromagnet, they develop into a magnetic supramolecular layer with spin-filtering properties; this could be the basis for a new approach to building molecular magnetic devices. Various types of molecular magnets carrying high localized spin have been studied as potential devices for information processing and storage, but it remains a considerable challenge to electronically couple to these spin centres. Moodera et al. have designed a phenalenyl derivative, essentially a graphene fragment, with the potential to act as an interface for the exchange of magnetic spin information in molecular spintronic devices. The graphene fragment has no net spin itself, but when deposited as a layer on a ferromagnet it transforms to produce a supramolecular magnetic film. The resulting nanoscale magnetic molecules, or memory 'bits', can be manipulated by external stimuli, and the resulting device exhibits an unexpectedly large magnetoresistance of 20% near room temperature. The use of molecular spin state as a quantum of information for storage, sensing and computing has generated considerable interest in the context of next-generation data storage and communication devices1,2, opening avenues for developing multifunctional molecular spintronics3. Such ideas have been researched extensively, using single-molecule magnets4,5 and molecules with a metal ion6 or nitrogen vacancy7 as localized spin-carrying centres for storage and for realizing logic operations8. However, the electronic coupling between the spin centres of these molecules is rather weak, which makes construction of quantum memory registers a challenging task9. In this regard, delocalized carbon-based radical species with unpaired spin, such as phenalenyl10, have shown promise. These phenalenyl moieties, which can be regarded as graphene fragments, are formed by the fusion of three benzene rings and belong to the class of open-shell systems. The spin structure of these molecules responds to external stimuli11,12 (such as light, and electric and magnetic fields), which provides novel schemes for performing spin memory and logic operations. Here we construct a molecular device using such molecules as templates to engineer interfacial spin transfer resulting from hybridization and magnetic exchange interaction with the surface of a ferromagnet; the device shows an unexpected interfacial magnetoresistance of more than 20 per cent near room temperature. Moreover, we successfully demonstrate the formation of a nanoscale magnetic molecule with a well-defined magnetic hysteresis on ferromagnetic surfaces. Owing to strong magnetic coupling with the ferromagnet, such independent switching of an adsorbed magnetic molecule has been unsuccessful with single-molecule magnets13. Our findings suggest the use of chemically amenable phenalenyl-based molecules as a viable and scalable platform for building molecular-scale quantum spin memory and processors for technological development.