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.　Graphical　Abstract:　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.[Figure　not　available:　see　fulltext.]　©　2023,　Shanghai　University　and　Periodicals　Agency　of　Shanghai　University.