The invention provides a high-strength/toughness magnesium lithium alloy and a preparation method thereof by an accumulative roll bonding process. The method comprises the following steps: a) carrying out homogenizing treatment on a smelted magnesium lithium alloy cast ingot; b) carrying out thermal deformation processing to obtain a magnesium lithium alloy plate; c) carrying out stress-relief annealing; d) cutting the plate for accumulative roll bonding into two pieces with equal size, and carrying out surface treatment; e) fixing the two Mg-Li alloy plates; f) rolling; g) repeating the roll bonding according to the steps d)-f) 4-6 times; and h) carrying out annealing treatment. The obtained alloy comprises the following components in percentage by mass: 7.5-9.5% of Li, 2.5-3.5% of Al, 0.5-1.5% of Zn, less than 0.03% of inevitable impurities (Fe, Cu, Ni, Mn and Si), and the balance of Mg. The magnesium lithium alloy is reinforced according to the specific alloying elements and proportioning thereof, and subjected to multipass accumulative roll bonding at proper temperature to refine the magnesium lithium alloy crystal grains, so that the alloy has higher strength on the premise of keeping favorable plasticity.