Layered double hydroxides (LDH) with highly flexible and adjustable chemical composition and physical properties have attracted tremendous attention in recent years. A series of LDH with different M (Mg, Zn, Mn)-Fe molar ratios were synthesized by the double titration co-precipitation method. The effect of the factors, including M (Mg, Zn, Mn) : Fe molar ratio, pH, and M-Fe LDH dosage, on the ability of the prepared M-Fe LDH to remove cationic methylene blue (MB) dye from aqueous solution were investigated. Results indicated that the removal efficiency of MB (10 mg/L) was the best at the M (Mg, Zn, Mn): Fe molar ratio of 3:1 by using 2.0 g/L of M-Fe LDH at pH 6.0 under 298.15 K. Mg-Fe LDH had the highest removal performance (71.94 mg/g at 298.15 K) for MB compared to those of the Zn-Fe and Mn-Fe LDH. Zn-Fe LDH with the smallest activation energy resulted in the fastest adsorption rate of MB. The pseudo-second-order model and Langmuir adsorption isotherm were also successfully applied to fit the theory of M-Fe LDH for removal of MB.