Advanced energy storage technology represented by lithium (Li)-ion batteries (LIBs) has revolutionized human life in recent years. The energy density of LIBs based on intercalation chemistry is approaching its theoretical limit after unremitting efforts for the past three decades. The state-of-the-art LIBs with graphite anode can only achieve an energy density lower than 300 Wh kg â1 . [1] This cannot satisfy the increasing demands for portable electronic devices, electric vehicles, and stationary energy storage systems. [2] Therefore, it is urgently called for next-generation batteries with a high energy density, long lifespan, and high safety performance. [3,4] Electrode material is of great importance in determining the energy density of batteries. [5] As the holy grail anode, Li metal possesses the ultrahigh theoretical specific capacity (3860 mAh g â1 ) and low potential (â3.04 V vs the standard hydrogen electrode). The promising feature renders Li metal anode to be an indispensable candidate for constructing next-generation high-energy-density batteries. [6] A high energy density of 400 or even 500 Wh kg â1 can be achieved with Li metal batteries (LMBs) matching Ni-rich LiNi x Co y Mn (1âxây) O 2 (0 < x, y <1), oxygen, or sulfur cathodes, etc. [7][8][9] However, the conversion chemistry and high reactivity of Li metal also bring great challenges to the design of robust LMBs with long lifespan and high safety. [10,11] Specifically, Li dendrite growth and infinite volume variation lead to unstable solid electrolyte interphase (SEI) on Li metal anodes, resulting in low Li utilization, capacity decline, and even safety risk, [12] severely hindering the practical applications of LMBs. [13][14][15] Recently, extensive strategies have been exploited to control the dendrite growth of Li metal anodes, including engineering electrolytes and additives, [16] designing 3D host structures, [17][18][19] constructing artificial SEI, [20,21] applying solid-state electrolyte (SSE), [22][23][24] and adjusting operation conditions. [25] A high Coulombic efficiency (>99.9%) and long lifespan (>1000 cycles) have been reported in the materials-level coin cells. [26][27][28] Notably, Li dendrite growth is primarily driven by the kinetical limitation of Li-ion diffusion near the electrolyte/electrode interface. Serious dendrite issues can be encountered under harsh operating conditions in pouch cells, considering the accelerated consumption of Li ions at large currents and high Lithium metal battery has been considered as one of the potential candidates for next-generation energy storage systems. However, the dendrite growth issue in Li anodes results in low practical energy density, short lifespan, and poor safety performance. The strategies in suppressing Li dendrite growth are mostly conducted in materials-level coin cells, while their validity in device-level pouch cells is still under debate. It is imperative to address dendrite issues in pouch cells to realize the practical application of Li metal batteries. This review prese...