A Universal Multiscale Ion–Electron Dual Regulation for on‐Demand All‐3D‐Printed High‐Voltage Full Batteries

Abstract To achieve on‐demand distribution of next‐generation batteries, battery manufacturing methods are shifting toward digital approaches, particularly 3D printing. Notably, 3D printing allows structurally tailored electrode architectures, thus offering tremendous advances in elevating battery energy storage behaviors, and a universal 3D‐printing approach with ion‐electron tuning capabilities remains imperative but challenging. In this work, a universal multiscale ion‐electron dual‐regulation strategy is proposed, leveraging LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM) as a typical active material, for all‐3D‐printed full batteries. By optimizing the ink formulations and digitally tailoring the electrode microstructures, on‐demand high‐loading electrode architectures are constructed with engineered networks. The resulting NCM‐centered networks exhibit a remarkable discharge capacity of 266.1 mAh g⁻ 1 , superior rate capability, and exceptional stability over 10,000 cycles. The excellent performance is attributed to the well‐tuned ion‐electron transport, which is further substantiated by simulation insights. Upon integration into full batteries, a remarkable capacity of 164.5 mAh g⁻¹ and 85.5% capacity retention after 5,000 cycles are achieved. This regulation strategy is also applicable for other battery materials, thereby establishing a universal and scalable route for 3D‐printed energy storage materials and devices. It represents an advancement for next‐generation digital, intelligent, and sustainable battery manufacturing.