Coffee post-processing drying eliminates moisture content, reduces fungal and microbe growth, and develops unique aroma and flavor compounds. Thai coffee producers use controlled-environment drying (CED) techniques to improve the quality and cupping scores of the coffee. This research investigated how different drying methods, including sun drying (SD), controlled-environment drying at 20–30 °C, 50–55% RH, and fast drying (FD) at 30–45 °C influenced the physicochemical characteristics of coffee undergoing dry (DP), washed (WP), and honey (HP) processing. Results showed that true density, moisture content, water activity, color, caffeine, trigonelline, chlorogenic acid, caffeic acid, sucrose, and fructose in green coffee beans were significantly affected (p < 0.05) by both drying technique and post-harvest processing. Drying techniques and processing directly impacted the characteristics of green (GCB) and roasted coffee beans (RCB). Findings suggested a correlation between CED, SD, and FD based on the physicochemical and biochemical properties and sugar contents of both green and roasted coffee beans.