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Intrinsic magnetic properties of two-dimensional (2D) nanomaterials, especially monolayer or few-layer inorganic ultrathin nanosheets, have been widely studied due to their own novel spin structures and special magnetic states induced by the quantum confinement of electrons. When the thickness reduces to the atomic-scale, 2D nanomaterials have extremely large specific surface area, providing abundant surface atoms and surface sites and therefore provide a way to modify surface structures and spin for efficiently engineering their intrinsic magnetic properties. In this chapter, we focus on recent research on strategies for realizing surface chemical modification and effectively engineer the intrinsic magnetic properties of inorganic 2D nanomaterials. We highlight recently reported regulation strategies, such as surface incorporation, defect engineering and structure modulation, which influence the intrinsic magnetic properties without destroying the pristine 2D freestanding structures that are vital for developing 2D ultrasensitive field-sensitive devices, spintronic devices and magnetocaloric materials.

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