Coffee is the world’s second most traded commodity and the most renowned drink worldwide. The increasing production of coffee has been accompanied by a rise in consumption, and consequent increment in the amount of spent coffee grounds (SCGs) remaining as a solid residue from coffee brewing. In view of the high content of biodegradable compounds, if disposed, SCGs will certainly need to be biostabilized, although they should preferably be exploited in a biorefinery chain scheme. A wide range of alternative options is available for use in recycling SCGs as a valuable resource: food additives, pharmaceutical components, bio-sorbents, bio-fuels, and bio-products. The option of producing biogas from SCGs was tested and lab-scale bio-methane potential experiments were performed using different substrate to inoculum (S/I) ratios, namely 0.5, 1, and 2. A S/I ratio of 2 was found to be the optimal condition, resulting in a methane yield of 0.36 m3CH4/kgVS.