The potential of microorganisms for enhancing carbon capture and storage (CCS) via mineral-trapping (where dissolved CO2 is precipitated in carbonate minerals) and solubility trapping (as dissolved carbonate species in solution) was investigated. The bacterial hydrolysis of urea (ureolysis) was investigated in microcosms including synthetic brine (SB) mimicking a prospective deep subsurface CCS site with variable headspace pressures [p(CO2)] of 13C−CO2. Dissolved Ca2+ in the SB was completely precipitated as calcite during microbially induced hydrolysis of 5−20 g L−1 urea. The incorporation of carbonate ions from 13C−CO2 (13C−CO32−) into calcite increased with increasing p(13CO2) and increasing urea concentrations: from 8.3% of total carbon in CaCO3 at 1 g L−1 to 31% at 5 g L−1, and 37% at 20 g L−1. This demonstrated that ureolysis was effective at precipitating initially gaseous [CO2(g)] originating from the headspace over the brine. Modeling the change in brine chemistry and carbonate precipitation after equilibration with the initial p(CO2) demonstrated that no net precipitation of CO2(g) via mineral-trapping occurred, since urea hydrolysis results in the production of dissolved inorganic carbon. However, the pH increase induced by bacterial ureolysis generated a net flux of CO2(g) into the brine. This reduced the headspace concentration of CO2 by up to 32 mM per 100 mM urea hydrolyzed because the capacity of the brine for carbonate ions was increased, thus enhancing the solubility-trapping capacity of the brine. Together with the previously demonstrated permeability reduction of rock cores at high pressure by microbial biofilms and resilience of biofilms to supercritical CO2, this suggests that engineered biomineralizing biofilms may enhance CCS via solubility-trapping, mineral formation, and CO2(g) leakage reduction.