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    and foldable films for display applications.
    22
    Although these
    NFC materials have good mechanical properties, the full
    mechanical potential of NFC was not fully achieved because the
    orientation distribution of NFC was random-in-the-plane or
    random-in-space.
    Several efforts to orient cellulose nanofibers and whiskers
    have been presented. Orientation has been reported in
    dispersions, films, and fibers. In a dispersion, cellulose
    microcrystals undergo spontaneous parallel arrangements in
    the form of a chiral nematic phase.
    23
    A magnetic
    24
    or electric
    25
    field can also orientate rodlike cellulose whiskers in the liquid
    state, and subsequent drying gives oriented films. Films of
    highly oriented cellulose whiskers have been reported by
    Received: November 29, 2011
    Accepted: January 18, 2012
    Published: January 18, 2012rotation of a glass vial containing aqueous dispersion of
    whiskers, followed by drying.
    26
    All-cellulose films (composite
    films of cellulose I and II) were cold drawn in the wet state to
    induce orientation in the drawing direction.
    27
    For fibers with
    oriented cellulose, wet spinning, hot drawing and electro-
    spinning have been used. Wet spinning has been used on wood
    cellulose nanofiber and tunicate whisker dispersions using
    acetone as a coagulation bath. The spinning rate and the nature
    of the starting dispersion was found to give different fiber
    structure (hollow or porous fibers).
    28
    Hot-drawing in the
    presence of a polymer matrix was used to obtain fibers with
    cellulose whiskers in a PVA matrix where both the PVA matrix
    and the whiskers showed a high degree of orientation.
    29
    Electrospinning also gives fibers with oriented whiskers in a
    polymer matrix. The electrospun fibers can be randomly
    assembled into a porous membrane, or aligned with a drum
    collector.
    30
    The starting point of the present study is NFC nanopaper,
    and this is a web-like network of cellulose nanofibrils.
    5,12
    The
    NFC orientation distribution is random-in-the-plane. Interest-
    ing properties include optical transparency,
    31
    smoothness,
    12
    low coefficient of thermal expansion,
    31
    good mechanical
    properties,
    5,12
    and possibilities for functionalization.
    21,32
    The
    nanopaper can be prepared by a water-based papermaking-like
    filtration procedure,
    5,12
    and therefore offers solvent-free
    preparation compared with regenerated cellulose films.
    Furthermore, the nanopaper consists of cellulose I type fibrils
    with better mechanical properties compared to cellulose II.
    33
    Suggested applications for NFC nanopaper includes films for
    packaging applications,
    5,6
    electronic display application22
    or as a
    substrate for nanocomposites preparation (e.g., by impregna-
    tion).
    34
    In this later application, an advantage would be to have
    orientation of NFC so that further tailoring of the mechanical
    properties becomes possible. For instance, it would be possible
    to prepare laminates based on oriented film “plies” stacked with
    varying orientation angle so that mechanical properties in
    different directions can be tailored.
    Cold drawing has already been used for preparation of all-
    cellulose films with preferred orientation.
    27
    The preparation
    steps of oriented all-cellulose films include partial dissolution of
    MCC in LiCl-DMAc solvent, gelation, washing, drying of the
    films, wetting of the dried films, stretching (cold drawing) of
    the wet films, and finally drying the films in stretched
    conditions. The drawn all-cellulose films presented excellent
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