Bottom‐Up Magnesium Deposition Induced by Paper‐Based Triple‐Gradient Scaffolds toward Flexible Magnesium Metal Batteries

The development of advanced magnesium metal batteries (MMBs) has been hindered by longstanding challenges, such as the inability to induce uniform magnesium (Mg) nucleation and the inefficient utilization of Mg foil. This study introduces a novel solution in the form of a flexible, lightweight, paper‐based scaffold that incorporates gradient conductivity, magnesiophilicity, and pore size. This design is achieved through an industrially adaptable papermaking process in which the ratio of carboxylated multi‐walled carbon nanotubes to softwood cellulose fibers is meticulously adjusted. The triple‐gradient structure of the scaffold enables the regulation of Mg ion flux, promoting bottom‐up Mg deposition. Owing to its high flexibility, low thickness, and reduced density, the scaffold has potential applications in flexible and wearable electronics. Accordingly, the triple‐gradient electrodes exhibit stable operation for over 1200 h at 3 mA cm−2/3 mAh cm−2 in symmetrical cells, markedly outperforming the non‐gradient and metallic Mg alternatives. Notably, this study marks the first successful fabrication of a flexible MMB pouch full cell, achieving an impressive volumetric energy density of 244 Wh L−1. The simplicity and scalability of the triple‐gradient design, which uses readily available materials through an industrially compatible papermaking process, open new doors for the production of flexible, high‐energy‐density metal batteries. A flexible paper‐based scaffold exhibiting gradient conductivity, magnesiophilicity, and pore size is fabricated using an industrially compatible papermaking process. This triple‐gradient design controls the Mg ion flux for bottom‐up deposition, facilitating superior cyclability. The high flexibility and minimal thickness of the scaffold align well with the emerging demand for flexible and wearable electronics, signaling a robust pathway for their advancement.