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Psychrophilic anaerobic digestion emerges as an appealing integrated solution for the management of agricultural waste, particularly for farmers in regions where the average temperature does not exceed 26 °C, as seen in coffee cultivation. Therefore, this study seeks to assess the biomethane potential of thermochemical-treated coffee husk through psychrophilic anaerobic digestion (C3-20 °C-w/pretreatment). To examine its viability, outcomes were compared with reactors operating at both mesophilic (C1-35 °C) and psychrophilic (C2-20 °C) conditions, albeit without the use of pretreated coffee husk. The C3-20 °C-w/pretreatment test demonstrated a 36.89% increase (150.47 NmL CH4/g VS; 161.04 NmL CH4/g COD), while the C1-35 °C test exhibited a 24.03% increase (124.99 NmL CH4/g VS; 133.77 NmL CH4/g COD), both in comparison to the C2-20 °C test (94.96 NmL CH4/g VS; 101.63 NmL CH4/g COD). Notably, the C3-20 °C-w/pretreatment trial yielded superior outcomes, accompanied by an associated energy output of 3199.25 GWh/year, sufficient to meet the annual energy demands of 494 residences. This marks an increase of 83 and 182 million residences compared to the mesophilic and psychrophilic AD of CH without pretreatment, respectively.