Scalable decarbonization efforts require the production of low-carbon hydrogen energy alternatives. Currently, more than 80% of hydrogen is produced via steam methane reforming (SMR) followed by water gas shift reaction (WGSR) pathway that produces significant CO2 emissions, regardless of the use of fossil or bio-derived methane. Hence, feasible pathways, particularly carbon mineralization, for post- and in-situ carbon removal integrated with H2 production are of significant interest, necessitating further explorations of their mechanistic insights. To eliminate the uncontrollability from compositional and morphological heterogeneity of naturally occurring minerals, we develop a novel synthesis pathway for potentially high-performance carbon sorbents with architected structures and morphologies, in which advanced synchrotron cross-scale X-ray scattering measurements are employed for in-depth mechanistic study. A significant but less-studied mechanism in carbon mineralization is the impact of amino acid salts, which potentially enhances CO2 dissolution via carbamate formation. To fill the knowledge gap, sodium glycinate solutions at different concentrations are applied in our research to explore their CO2 capture performance at low-temperature regimes (<100 °C) and ambient pressure. The remarkable carbon mineralization enhancement at moderate conditions confirms the feasibility of amino acid salt solutions, advancing an energy-efficient approach for post-H2 production carbon removal after gas cooling. Furthermore, carbon mineralization proceeding under the same conditions as WGSR (200-300 °C, 20 atm) is investigated in water and NaHCO3 solution to address the challenge of post-H2 production carbon removal without gas pretreatment. The observations reveal correlations between dissolution behavior and carbon mineralization performance under high temperatures and pressures, providing transformative insights into optimizing the reaction configuration for high-temperature carbon mineralization. Consequently, a seldom-reported enhanced WGSR coupled with in-situ aqueous carbon mineralization is discussed. Thermodynamic models of the multiphase approaches are derived to predict the enhancements in CO conversion via WGSR with different carbon sorbents. The experimental results exhibit great consistency with the thermodynamic predictions, indicating effective H2 yield improvement and CO2 emissions suppression. These findings emphasize the significance of in-situ carbon mineralization for H2 production approaches and further advance the understanding of their interaction, which is a step forward in sustainable hydrogen fuel harness with net-zero carbon emissions.