Growing environmental awareness and depleting fossil resources pose an emerging quest for lightweight materials with outstanding mechanical properties and economic production from sustainable resources that are biodegradable, carbon neutral, and safe. Super-strong yet lightweight anisotropic nanocellulose films are demonstrated by a cellulose DP protection strategy, exhibiting a tensile strength up to 1.13GPa. The high strength and low density of the nanocellulose films renders the highest specific strength of 820 MPa cm 3 g À1 among any known natural polymers and some strong metals.

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A highly transparent cellulose film with a high built-in haze is emerging as a green photonic material for optoelectronics. Unfortunately, attaining its theoretical haze still remains a challenge. Here, we demonstrate an all-cellulose composite film with a 90.1% transmittance and a maximal transmission haze of 95.2% close to the theoretical limit (∼100%), in which the entangled network of softwood cellulose fibers works as strong light scattering sources and regenerated cellulose (RC) with undissolved fibril bundles functions as a matrix to simultaneously improve the optical transparency and transmission haze. The underlying mechanism for the ultrahigh haze is attributed to microsized irregularities in the refractive index, arising primarily from the crystalline structure of softwood fibers, undissolved nanofibril bundles in RC, and a small number of internal cavities. Moreover, the resulting composite film presents a folding resistance of over 3500 times and good water resistance, and its application in a perovskite solar cell as an advanced light management layer is demonstrated. This work sheds light on the design of a highly transparent cellulose film with a haze approaching the theoretical limit for optoelectronics and brings us a step further toward its industrial production.

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