Disclosed herein is a method of depositing a nanolaminate film for next-generation non-volatile floating gate memory devices by atomic layer deposition. The method includes the steps of: introducing a substrate into an atomic layer deposition reactor; forming on the substrate a first high-dielectric-constant layer by alternately supplying an oxygen source and a metal source selected from among an aluminum source, a zirconium source and a hafnium source; forming on the first high-dielectric-constant layer a nickel oxide layer by alternately supplying a nickel source and an oxygen source; and forming on the nickel oxide layer a second high-dielectric-constant layer by alternately supplying an oxygen source and a metal source selected from among an aluminum source, a zirconium source and a hafnium source. The nanolaminate film deposited according to the method shows good memory window characteristics compared to those of memory devices fabricated using nanocrystal floating gates according to the prior physical vapor deposition methods, and thus can be applied to non-volatile floating gate memory devices.