The invention discloses a process for preparing acicular, flake nano single crystal magnesia-alumina hydrotalcite Mg6Al2(OH)16C.4H2O, and the prepared Mg6Al2(OH)16CO3.4H2O is used as a flame retardant of power electronic devices. Acicular components comprise 0.06-1.41 mol/L crystal magnesium chloride, 0.02-0.47 mol/L aluminum salt, 0.3-4.5 mol/L sodium hydroxide and 0.094-1.368 mol/L sodium carbonate, and flake components are added with modifier basing on the above components. The invention has the process steps that the crystal magnesium chloride and the sodium hydroxide are firstly dissolved in deionized water and heated and stirred, and then the aluminum salt and sodium carbonate are added into the solution, the deionized water and the sodium hydroxide are added every 20 minutes during reaction, the time of reaction is 0.5-2 hours, and the solution is cooled until room temperature and is washed, filtered and dried. The crystal morphology of the prepared acicular nano single crystal magnesia-alumina hydrotalcite is that the diameter is 10-20 nanometer, the length is 60-130 nanometer, the diameter is 25-80 nanometer, and the length is 200-500 nanometer. The crystal morphology of the flake nano single crystal magnesia-alumina hydrotalcite is that the thickness is 10-20 nanometer, the diameter is 50-100 nanometer, the thickness is 20-30 nanometer, and the diameter is 60-200 nanometer. The process for preparation of the invention has short period and simple process, is prepared at atmospheric pressure, and is suitable for industrial production.