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The tung tree (<i>Vernicia fordii</i> Hemsl.), as a woody oilseed crop, has been cultivated in China for thousands of years, and its leaves are rich in cellulose and proteins. The tung leaf is an alternative raw material for the traditional ethanol fermentation of food crops. In this work, the effects of the simultaneous saccharification fermentation of tung leaves at different substrate concentrations on gas production characteristics, reducing sugars, pH, oxidation–reduction potential (ORP), and ethanol yield were investigated during bioethanol production. In addition, the effect of the initial fermentation pH on the ethanol fermentation of tung leaves was explored. The results showed that during bioethanol production from tung leaves, the pH of the fermentation broth showed a continuous decreasing trend. Moreover, the ORP showed a decreasing trend and then rebounded, and the concentration of reducing sugars initially increased and then decreased. The optimal ethanol yield of 4.99 g/L was obtained when the substrate concentration was 100 g/L. Changes in the initial pH have little effect on yeast activity, but such changes can affect the yeast cell wall structure and substance transport, leading to differences in the ethanol yield. When the initial pH is 7, the maximum ethanol yield is 5.22 g/L. The experimental results indicate that the utilization of tung leaves for bioethanol production has a good potential for development.