The behavior of amorphous cellulose model thin films upon heat treatment is investigated. Upon heat treatment, a structural rearrangement in the films from a featureless to a fibrillar structure is observed which correlates with the regeneration time and total cellulose content as proven by atomic force microscopy and X-ray photoelectron spectroscopy. ATR-IR spectroscopy proves the presence of stronger hydrogen bonds in the heat treated surfaces which originate from a reorganization of the cellulose chains and pore structure. The rearrangement is accompanied with an increased surface hydrophobicity, a reduced swelling capacity and a reduction in the water content of the films. An increase in crystallinity of the films is not observed.
