Hybrid devices based on spin‐crossover (SCO)/2D heterostructures grant a highly sensitive platform to detect the spin transition in the molecular SCO component and tune the properties of the 2D material. However, the fragility of the SCO materials upon thermal treatment, light irradiation, or contact with surfaces and the methodologies used for their processing have limited their applicability. Here, an easily processable and robust SCO/2D hybrid device with outstanding performance based on the sublimable SCO [Fe(Pyrz)2] molecule deposited over chemical vapor deposition (CVD) graphene is reported, which is fully compatible with electronics industry protocols. Thus, a novel methodology based on growing an elusive polymorph of [Fe(Pyrz)2] (tetragonal phase) over graphene is developed that allows a fast and effective light‐induced spin transition in the devices (≈50% yield in 5 min) to be detected electrically. Such performance can be enhanced even more when a flexible polymeric layer of poly(methyl methacrylate) is inserted in between the two active components in a contactless configuration, reaching a ≈100% yield in 5 min.

Among the different types of switchable molecular compounds, sublimable Fe(II) SCO molecules provide a suitable platform to develop smart devices that respond to external stimuli. Here we report the synthesis,...

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