The efficient exfoliation of mica, a naturally layered material, into two-dimensional (2D) nanosheets has received much attention due to its low price, good chemical stability, and better shielding function against UV light. However, fast and simple exfoliation of mica in a large-scale face a great challenge. In this work, we developed a simple and effective method for obtaining OH−functionalized mica nanosheets (MNs). The process involved calcination, plasma treatment, and ultrasonic exfoliation, resulting in a yield of 7.535%. Furthermore, the effects of sonication time, solvent type, and particle sizes of mica were investigated. The conditions for the preparation of MNs were determined: mica calcination, plasma treatment, and sonication in ethanol for 5 h. XPS and FT−IR demonstrated that more hydroxyl groups were introduced to mica after the plasma treatment, which facilitated the exfoliation of mica.