Sensory evaluation, in vitro antioxidant activities and main compounds of coffee water-extract, coffee liqueur (CL) and coffee-ground liqueur (CGL) were investigated to consider their industrialization. Sensory evaluation showed that all groups of CGL without 25% CGL (3 month) were relatively higher than CL groups. Total phenolic compounds and in vitro antioxidant activities such as 1,1-diphenyl-2picryl-hydrazyl (DPPH) radical scavenging activity and ferric reducing/antioxidant power (FRAP) were also performed. The group of 35% CGL had higher total phenolic compounds than others, and the result of DPPH radical scavenging activity was similar to that of total phenolic compounds. In addition, 35% CGL is comparable to the FRAP of coffee water extract (CE). Qualitative and quantitative analysis using high-performance liquid chromatography (HPLC) were performed, and chlorogenic acid as a ployphenolic compound and caffeine as a nonpolyphenolic compound were detected in all samples. Moreover, the HPLC analysis showed that CGLs contain a larger amounts of chlorogenic acid (difference of 0.3~10.5%) and also greater amounts of caffeine (difference of 10.0~18.2%) more then CE. Consequently, these results suggest that coffee-ground as coffee by-products could be used as commercially available food substances because of its physiological molecules remained.