The growth structure of MgF2 and NdF3 films grown on polished CaF2(111) substrates deposited by molecular beam deposition has been investigated using transmission electron microscopy (TEM) of microfractographical and surface replications as well as cross-sectional TEM, atomic force microscopy, packing density, and absorption measurements. It has been shown that by taking advantage of ultrahigh vacuum environments and a special stratification property of MgF2 and NdF3 films, the preparation of nanocrystalline films of high packing density and low optical absorption is possible at a substrate temperature of 425 K.