The voltammetric behavior, nucleation mechanism, and electrodeposition of zinc were carefully studied in hydrophobic roomtemperature ionic liquid 1-butyl-1-methylpyrrolidinium bis((trifluoromethyl)sulfonyl)imide (RTIL [BMP][TFSI]). The Zn(II) species were introduced via the anodic dissolution of Zn, or the addition of Zn(TFSI) 2 and ZnCl 2 , respectively. Unexpectedly, ZnCl 2 shows a high solubility in [BMP][TFSI] where most metal chlorides are almost insoluble. For electrodeposition, ZnCl 2 hence can be used as a cheaper and time-saving alternative of the Zn(II) source. Two Zn salts show obviously different voltammetric behavior, which may result from the different Zn(II) species formed. Two redox couples of Zn(II) are observed in ZnCl 2 solutions but there is only one redox couple in Zn(TFSI) 2 solutions. Many phenomena imply that two Zn(II) species, one is partially Cl-coordinated and the other one is TFSI-coordinated, are produced from ZnCl 2 . The surface morphology of Zn deposits prepared from the two Zn salts at 80 • C is not distinguishable but apparently changed with the electrodepositing potential. Similarly, the nucleation mechanism is independent of the Zn salts, and a 3-dimensional (3D) progressive nucleation with diffusion controlled growth is observed. Oppositely, the deposition/stripping efficiency of Zn is significantly influenced by the source of Zn(II); a much higher efficiency is observed in the Zn ( Zinc is an important industrial metal regarding to the usage in corrosion-resistance coatings, 1 in energy storage devices such as Zn batteries, 2,3 and electrocatalysis. 4 Regardless of which application, electrodeposition of Zn is involved, and the relevant study is hence important. For electrodeposition of metals, the choice of the electrolytes is always crucial to the surface morphology of the electrodeposits, the current efficiency, the stability of the electrodeposits in the electrolytes, and the impact to the environment.Ionic liquids (ILs), including deep eutectic solvents (DESs), have been recognized as better electrolytes than organic or aqueous ones for the electrodeposition of metals, including Zn, 5,6 offering an alternative to toxic and/or corrosive additives such as cyanide and acid chloride. Moreover, if aprotic ILs are used, hydrogen evolution, which is usually encountered in the electrodeposition of active metals such as Zn in aqueous solutions, can be significantly suppressed, leading to a more controllable surface morphology and higher current efficiency. Zn has been successfully electrodeposited from the traditional Lewis acidic ILs, 7-10 the air-and water-stable ILs, 3,[11][12][13][14][15][16][17][18][19] To search a common source of Zn ions and a suitable IL for the electrodeposition of Zn metal, however, is still important.The hydrophobic RTIL 1-butyl-1-methylpyrrolidinium bis ((trifluoromethyl)sulfonyl)imide ([BMP][TFSI]) has been widely used for the study of metal and alloy electrodeposition in view of various advantages, such as wide electrochemical window, wide tempera...