Cellulose limited by fusibility and solubility is impossible to be directly thermoformed, of which the existing progress crucially relies on larger liquids, making it hard to achieve a direct all-green manufacture. Here, we propose an innovative strategy that the surface molecular chains of cellulose nanospheres are activated at 100 °C and intertwined under 500 MPa because of the high molecular activity on the surface of nanospheres and the reduction of activation energy after ball-milling. It is confirmed that only physical changes are involved, according to infrared spectrum. Results show that applicable mechanical properties (hardness and modulus reach 0.44 and 9.66 GPa, respectively) are successfully obtained. Simultaneously, the optimum optical performance of all-cellulose substrate reaches more than 80 % at visible light. Combined with their intrinsic properties, these cellulose-based products could be potentially utilized as biomass substrates. Therefore, our innovative strategy opens up a door for the direct thermoforming of cellulose.

受易熔性和溶解性限制的纤维素不可能直接热成型，其中现有的进展至关重要地依赖于较大的液体，因此很难实现直接的全绿色生产。在这里，我们提出了一种创新的策略，由于纳米球表面的高分子活性和球磨后的活化能降低，纤维素纳米球的表面分子链在100°C时被活化并在500 MPa下缠绕在一起。已经证实，根据红外光谱，仅涉及物理变化。结果表明，成功获得了适用的机械性能（硬度和模量分别达到0.44和9.66 GPa）。同时，全纤维素底物的最佳光学性能在可见光下达到80％以上。结合它们的固有特性，这些基于纤维素的产品可以潜在地用作生物质底物。因此，我们的创新策略为纤维素直接热成型打开了一扇门。