Cellulose solution and nanocellulose were prepared from corn straw and wheat straw and then used to fabricate an all-cellulose nanocomposites film (ANF). The crystal structure (CS) of ANFs was analyzed by X-ray diffraction (XRD) and Fourier transform infrared spectrometry (FTIR). Cellulose-I and cellulose-II were found to coexist within regenerated cellulose films (RCF) and ANFs. With the change of nanocellulose content, the proportions of cellulose-I and cellulose-II changed. Cellulose transformation was found to depend on the raw material and the preparation method. When cellulose solution was prepared from corn straw that had been extracted, the cellulose type tended to be transformed from cellulose-I to cellulose-II; the proportion of cellulose-I showed a tendency to increase when nanocellulose content exceeded 1.5%. When the dissolved cellulose had been treated by an acid-alkali method, the results did not follow a clear pattern. However, when cellulose solution was prepared from wheat straw, under extraction method, the cellulose type tended to transform from cellulose-I to cellulose-II; under acid-alkali method, cellulose-I did not follow a clear pattern with nanocellulose content. Though the small amount of nanocellulose can’t dominate the content of cellulose-I, it could cause an increase in disorder of the cellulose matrix.