Li metal anodes have attracted tremendous attention in the last decade because of their high theoretical capacities and low electrochemical potentials. However, until now, there has only been limited success in improving the interfacial and structural stabilities and in realizing the highly controllable and large-scale fabrication of this emerging material; these limitations have posed great obstacles to further performing fundamental and applied studies in Li metal anodes. In this review, we focus on summarizing the existing challenges of Li metal anodes based on the leap from coin cells to pouch cells and on outlining typical methods for designing Li metal anodes on demand; we controllably engineer their surface protection layers and structure sizes by encapsulating structured Li metal inside a variety of synthetic protection layers. We aim to provide a comprehensive understanding and serve as a strategic guide for designing and fabricating practicable Li metal anodes for use in pouch batteries. Challenges and opportunities regarding this burgeoning field are critically evaluated at the end of this review.Li metal anode has attracted tremendous attention in the last decade because of its high theoretical capacity and low electrochemical potential. However, till now, there is only limited success in improving its interface stability and structure stability, as well as realizing the highly controllable and large-scaled fabrication of this emerging material, posing great obstacles to further promoting its fundamental and applied studies. In this review, we focus on summarizing the existing challenges of Li metal anode based on the leap from coin cells to pouch cells and outlining the typical solutions for designing Li metal anode on-demand through controllably engineering its surface protection layer and structure size, which trend is encapsulating structured Li metal inside a variety of synthetic protection layer. We aim to provide a comprehensive understanding and serve as a strategic guidance for designing and fabricating practicable Li metal anode using in pouch batteries. Challenges and opportunities regarding this burgeoning field are also critically evaluated at the end of this review.