Layered double hydroxide (LDH) single-layer nanosheets were traditionally prepared through a multi-step exfoliation process which is very time-consuming and of low efficiency. Herein we report the preparation of LDH single-layer nanosheets through a facile direct synthesis method. By introducing a layer growth inhibitor, one can directly synthesize LDH single-layer nanosheets instead of LDH layered compounds. The inhibitor weakens the interactions between neighboring layers, thus preventing the interlayer growth. This investigation on blocking interlayer growth by weakening interlayer interactions to obtain inorganic single-layer nanosheets opens a new route for the synthesis of 2-dimensional materials.