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The application of lithium (Li) metal anodes in rechargeable batteries is hindered by Li dendrite growth during Li deposition and low Li Coulombic efficiency (CE), where the nonaqueous electrolyte plays a critical role. In this work, the effects of different carbonate solvents and Li salts on Li deposition morphology and CE were systematically investigated. Typically, cyclic carbonates favor the formation of uniform Li films and improve Li CE more than linear carbonates do. Several specific cyclic carbonates that are conventionally used as solid electrolyte interphase (SEI) formation additives in Li-ion batteries can also improve the CE of Li anodes. Furthermore, among the nine electrolyte salts studied, LiAsF6 and lithium bis(oxalato)borate (LiBOB) lead to the highest CE. LiBOB also leads to better uniformity of deposited Li than other salts do. Considering the better safety of LiBOB as compared to LiAsF6, LiBOB is a promising salt for rechargeable Li metal batteries with high CE. By combining the best electrolyte solvent/salt that can lead to high CE with novel electrolyte additives that can prevent dendrite formation, it is possible to find an electrolyte that not only prevents Li dendrite formation but also leads to high CE during Li deposition/stripping processes. [ABSTRACT FROM AUTHOR]