This study explores the use of bentonite to enhance biological biogas upgrading in a bubble reactor (BR) operated under mesophilic conditions (39 ± 1 °C). The experimental setup consisted of a 2 L vertically oriented BR (height to diameter ratio 16:1) fed with a synthetic gas mixture (60% H2, 15% CO2, 25% CH4, v/v) at a gas recirculation rate of 4 L LR⁻¹ h⁻¹. The aim was to overcome hydrogen’s low gas-liquid mass transfer rate while avoiding the operational challenges typically associated with trickle-bed reactors (TBRs). Bentonite increases the density and hydrostatic pressure of the liquid medium, and likely alters its rheology, thereby extending the gas-liquid contact time without requiring elevated pressures or intensive gas recirculation. Additionally, bentonite is expected to provide microstructural support that promotes the formation of biofilm-like communities, creating favorable microenvironments for hydrogenotrophic methanogens. As a clay-based additive, bentonite may also contribute to improved process stability through adsorption of inhibitory compounds, enhanced bio-mass retention, and pH buffering. Under mesophilic conditions, the bentonite-modified BR achieved a methane production rate of 2.17 ± 0.06 L CH4 LR⁻¹ d⁻¹ at a gas retention time of 1.49 h, with methane purity reaching 96.25%. In comparison, a previously reported mesophilic BR operated under identical reactor configuration and operating conditions but without bentonite exhibited substantially lower methane production rates, supporting the beneficial role of bentonite in biological methanation. The findings highlight bentonite’s potential dual role -physical and biological- in improving process efficiency and stability in biological methanation.