In this work, we report the preparation of novel leaflike Cu-O-Sn nanosheet catalysts for the Rochow reaction. The catalysts were synthesized via a facile hydrothermal approach using CuSO4 center dot 3H(2)O and SnCl4 center dot 5H(2)O as the precursors, but without the use of any template. When used for the Rochow reaction to synthesize dimethyldichlorosilane (M2), the as-prepared 0.1 wt.% Cu-O-Sn nanosheet exhibited a much higher M2 selectivity (93.3%), Si conversion (68.4%), and stability than the catalysts of CuO or SnO2 alone, the Cu-O-Sn catalysts with different compositions, and the commercial catalysts. The samples were characterized by X-ray diffraction, transmission electron microscopy, scanning electron microscopy, atomic force microscopy, Raman spectroscopy, X-ray photoelectron spectroscopy, and temperature-programmed reduction analyses. Surface segregation of Sn was observed, and the quantities of chemisorbed oxygen species and cation vacancies were well correlated with the activity of the catalysts. It is concluded that small crystal size, high chemisorbed oxygen species concentration, more cation vacancies, and strong interaction between Cu and Sn are responsible for the excellent catalytic performance of 0.1 wt.% Cu-O-Sn catalyst. (C) 2016 Elsevier Inc. All rights reserved.