The hydrate-based method enhances oceanic CO2 storage capacity and is deemed beneficial for controlling greenhouse gas emissions. However, the non-uniform CO2 hydrate crystal interface in the sub-seabed storage layer acts as a barrier, slowing down mass transfer kinetics. This work employed in-situ nuclear magnetic resonance (NMR) technology to compare three different pressure adjustment strategies and observe CO2 bubble dispersion after hydrate dissociation, secondary nucleation, and crystal growth mechanism, along with pore water changes. The presence of micro/nano CO2 bubbles with high internal pressure and high specific surface area in the dissociation liquid significantly accelerated secondary micro-structural phase transition rates. The optimal hydrate-based CO2 storage efficiency reached up to 81.7 %. Moreover, the secondary formation of CO2 hydrates distributed more uniformly within the large, medium, and small pores and led to a significantly increased residual water conversion rate (reaching up to 88 %) in medium pores. The post-secondary formation of high-density hydrates resulted in low fluid mobility (T1/T2 mostly distributed in the range of 0 ∼ 10) and exhibited a mixed wettability state between pore fluids. Utilizing the “memory effects” of CO2 hydrate effectively overcame late-stage mass transfer barriers of solid hydrates films. Our findings extend the understanding of CO2 hydrate formation kinetics under pressure adjustment strategies.