As a methanation tool, two-dimensional (2D) carrier-loaded Ni has attracted the attention of many researchers. We successfully prepared 2D MgAl layered double oxides (LDO) carriers via flash nanoprecipitation (FNP). Compared to the LDO samples prepared by conventional co-precipitation (CP), the 2D MgAl-LDO (FNP) has more oxygen vacancies and more exposed active sites. The Ni/MgAl-LDO (FNP) catalyst demonstrates a CO conversion of 97%, a CH4 selectivity of 79.8%, a turnover frequency of 0.141 s−1, and a CH4 yield of 77.4% at 350 °C. The weight hourly space velocity was 20,000 mL∙g−1∙h−1 with a synthesis gas flow rate of 65 mL∙min−1, and a pressure of 1 atm. A control experiment used the CP method to prepare Ni/MgAl-LDO. This material exhibits a CO conversion of 81.1%, a CH4 selectively of 75.1%, a TOF of 0.118 s−1, and a CH4 yield of 61% at 450 °C. We think that this FNP method can be used for the preparation of more 2D LDO catalysts.