The effects of dry processing and maturity on antioxidant activity, total phenolic content, total procyanidins, and identity of phenolic compounds in coffee leaves were evaluated. Fresh coffee leaves were tray-dried at 40 °C for 8 h before total phenolic content, total procyanidins, and antioxidant activity were analyzed. The drying process significantly (p < 0.05) improved the release of total phenolic content and total procyanidins compared with the fresh leaves. The results showed that the young leaves exposed to drying processes had the highest total phenolic content, total procyanidins, and DPPH radical scavenging activity. Therefore, the effect of different drying temperatures (30, 40, and 50 °C) in the young leaves were further analyzed. The results indicated that DPPH radical scavenging activity, total phenolic content, and total procyanidins were increasingly generated when exposed to an increase in drying temperatures, whereby the highest bioactivity was evident at 50 °C. The DPPH radical scavenging activity of the coffee leaf teas was significantly correlated with total phenolic content and total procyanidins. Identification of Coffea arabica L. bioactive compounds by LC-MS showed the presence of catechin or epicatechin, mangiferin or isomangiferin, procyanidin B, caffeoylquinic acids (CQA), caffeine, quercetin-3-O-glucoside, procyanidin C, rutin, and 3,4-diCQA. Coffea arabica L. leaf tea was confirmed to be a potential functional food rich in phenolic compounds with strong antioxidant activity.