The objective of this work was to investigate the efficiency and factors impacting of removal Cr(VI) from wastewater by layer double hydroxide synthesizing in situ. Principle of the method may be described as follow: Mg2+ and Al3+ hydrolysis and forms Mg/Al-LDH by adding Mg2+, Al3+ and NaOH into wastewater containing Cr(VI), Cr(VI) anions are selectively intercalated into interlayer of LDH to balance positive structural charge. While Mg2+ and Al3+ co-precipitates and forms LDH, the Cr(VI) in wastewater is removal by settle of LDH synthesizing in situ, which are confirmed by analysis of X-ray diffraction on settle and chemical analysis on aqueous. The results indicate that factors of impacting on efficiency of removal Cr(VI) include in amount of adding Mg2+ and Al3+, Mg/Al ratio, pH and concentration of Cr(VI) in wastewater. The maximal removal efficiency of Cr(VI) can be reached when pH values are between 8.5 and 9, and Mg/Al ratios are between 1:1 and 2:1, meanwhile, Mg and Al added can be taken good use of. This technology has present extraordinary efficiency of wastewater treatment.