The invention relates to nano thin sheet assembled nickel-iron hydroxide multistage microspheres and a preparation method thereof. With urea as an alkali source, with trisodium citrate as a complexing agent and with water and n-butyl alcohol as a reaction solvent, chemical solution mixed solvent heat is used for preparing the single or double layer nano sheet assembled layered double hydroxides NiFe-LDHs multistage microspheres. Firstly, a nickel salt, an iron salt, an alkali source and trisodium citrate are dissolved in the mixed solvent, and a reaction solution is prepared; and then the prepared reaction solution is treated under a solvothermal condition, and thus the regular-morphology single or double layer nano sheet assembled layered double hydroxides NiFe-LDHs multistage microspheres are obtained. Compared with the prior art, the method is simple, is low in cost, can synthesize the nickel-iron hydroxides multistage microspheres on large scale, and the nano sheet has the thickness of less than 2 nm.