Modified sericite mica was prepared by combining the intercalation of cetyltrimethylammonium bromide (CTAB) through ion exchange and surface modification of 3-aminopropyltriethoxysilane (KH550) with the following steps: high-temperature activation of sericite mica, acid activation, sodium modification, LiNO3 treatment, the ion-exchange intercalation of the cetyltrimethylammonium cation (CTA+) and surface modification of KH550. High-temperature activation was the most critical step for the modified sericite mica, and the number of hydroxyl groups of mica under high temperature directly affected the surface modification of KH550. The effects of various activation temperatures on the surface modification of sericite mica were investigated. The structure of activated sericite mica was intact when activation temperature was 600°C or 700°C, and the surface modification of sericite mica was not affected. The structure of activated sericite mica was partially destroyed at 800°C. The optimal temperature for activating sericite mica was 700°C. The structure and morphology of modified sericite mica were characterized by Fourier-transform infrared spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, scanning electron microscopy, Brunauer–Emmett–Teller (BET) analysis and loose bulk volume. The KH550 could not only chemically graft onto the surface of sericite mica, but also enter into the interlayer through electrostatic attraction after its end amino group was protonated. The interlayer spacing of modified sericite mica increased to 3.22 nm, indicating that it might be an excellent layered silicate for preparing clay–polymer nanocomposites.