Lightweight polymer composites promise incredible applications in aerospace, seaprobes, and medical apparatus. However, their performance is generally limited by a trade-off between mechanical strength and toughness. Herein, a crystallinity mitigating strategy driven by highly aligned bamboo macrofibers embedded in a polycaprolactone polyol (PCL) matrix for producing ultrastrong and tough lightweight polymer composites is proposed. The embedded bamboo macrofibers have oxygen-containing functional groups on the fiber surface, that can interact with functional groups (ester and hydroxyl groups) ...