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Layered double hydroxides (LDHs) have received extensive attention in many fields such as catalysis, environmental management and medical applications. Typically, expensive soluble metal salts are commonly used as the starting materials for the synthesis of LDHs. Here, we report a novel synthesis route for Mg/Al-LDH by using inexpensive basic magnesium carbonate as the starting material. X-ray diffraction (XRD) and solid-state nuclear magnetic resonance (ssNMR) data show that LDHs with rich defects are formed rapidly at room temperature and good crystallinity can be obtained after further hydrothermal treatment. These results provide a simple, rapid and green preparation method for LDHs.