2,3-Dialdehyde cellulose (DAC) of a high degree of oxidation (92% relative to AGU units) prepared by oxidation of microcrystalline cellulose with sodium periodate (48 °C, 19 h) is soluble in hot water. Solution casting, slow air drying, hot pressing, and reinforcement by cellulose nanocrystals afforded films (∼100 μm thickness) that feature intriguing properties: they have very smooth surfaces (SEM), are highly flexible, and have good light transmittance for both the visible and near-infrared range (89-91%), high tensile strength (81-122 MPa), and modulus of elasticity (3.4-4.0 GPa) depending on hydration state and respective water content. The extraordinarily low oxygen permeation of <0.005 cm3 μm m-2 day-1 kPa-1 (50% RH) and <0.03 cm3 μm m-2 day-1 kPa-1 (80% RH) can be regarded as a particularly interesting feature of DAC films. The unusually high initial contact angle of about 67° revealed a rather low hydrophilicity compared to other oxidatively modified or unmodified cellulosic materials which is most likely the result of inter- and intramolecular hemiacetal and hemialdal formation during drying and pressing.