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Coffee is one of the most consumed commodities globally, and its harvests generate large quantities of wood waste with low industrial value. This study aimed to explore the potential of residual Coffea arabica wood to produce lignocellulose microfibrils and lignocellulose nanofibrils (LCMF/LCNF) and biodegradable films with possible application in packaging. The fibers were treated with 5% NaOH and fibrillated in an ultrarefiner until they formed a gel. The resulting suspensions were used to create films whose physical, morphological, optical, and mechanical properties were analyzed. The NaOH treatment removed extractives and exposed hemicelluloses, allowing the gel point to be reached with just seven passes through the ultrarefiner, saving energy (~4700 kWh/t). More than 65% of the fibers had diameters of less than 100 nm and little sedimentation after 8 h. The films were flexible, thin (24.5 µm), with a high density (~1100 kg/m3) and good resistance to grease, as well as a water vapor permeability of ~1230 g/m2/day, suitable for packaging bread, fruit, and vegetables. However, the higher wettability of the surface may limit its use in humid environments. The films showed moderate tensile strength (~25 MPa) but low puncture resistance (~7 N mm), making them suitable for biodegradable packaging. [ABSTRACT FROM AUTHOR]