The price of raw material, energy demand in the pretreatment step, and enzyme usage rate are the major cost factors in the process of converting biomass to bioethanol. Unwashed furfural residues (FRs) possess great potential for application in bioethanol production. Surfactant addition is an effective method to enhance the fermentation rate. In this study, unwashed FRs were used directly as raw materials to produce bioethanol. Tea-seed cake (TSC), tea seed residues that contained protein and saponin, was added in the simultaneous saccharification and fermentation (SSF) process. The effect of TSC dosage on SSF was compared. TSC was added at the dosage of 10 g/L, which resulted in a final ethanol yield of 87.2%. However, a high concentration of TSC could induce cytotoxicity in yeast. The surface tension (approximately 33.92 mM/m) at SSF using TSC-medium was much lower than that of other fermentation systems (about 64.67 mN/m). Further contact angle testing showed that TSC-medium (21.7°) had better wetting capacity than FRs (45.6°). This study provided a proposed process strategy that SSF with the addition of TSC could be a minimum consumption of chemicals and enzymes for future cellulosic ethanol production process.