“…Bistable materials possessing two different states of physical channels, such as optical, electrical, magnetic, and mechanical properties, have attracted extensive concentration due to their great potential to realize seamless integration of multifunctional properties in one single device. − Among them, dielectric and nonlinear optical properties with bistable characteristics often exist in many functional materials, such as ferroelectrics, ferroelastics, ferromagnets, etc. − The bistability in many physical channels greatly improves the flexibility to control and retrieve the alternativity of the signal status. Some organic radicals with bistabilities in multiphysical channels, such as magnetism, conductivity, color, and IR transmittance due to the structural phase transition, were reported. ,− Nitroxyl radicals were usually designed as bistable magnetic materials arising from a radical/dimer interconversion (Figure a). − However, nitroxyl radicals with other bistable optoelectronic physical properties besides magnetism are rarely found as bistable multifunctional materials. Owing to the relatively high stability of nitroxyl radicals, ,, it is well worth excavating their bistability in other physical channels besides magnetic channels.…”