Investigating the immobilization of CO2, previous basalt-water-CO2 interaction studies revealed the formation of carbonates over a short period, but with the extensive formation of secondary silicates (SS). The mechanisms involved in these processes remain unresolved, so the present study was undertaken to understand secondary mineral formation mechanisms. XRPD and Rietveld refinement data for neo-formed minerals show a drastic decrease in the Ca-O bond length, with the calcite structure degenerating after 80 h (hours). However, SEM images and EDS data revealed that a longer interaction time resulted in the formation of chlorite and smectite, adjacent to basalt grains which prevent basalt-water-CO2 interaction to form carbonates, thus restricting carbonate formation. As a result of this, the CO2 mineralization rate is initially high (till 80 h), but it later reduces drastically. It is evident that, for such temperature-controlled transformations, low temperature is conducive to minimizing SS surface coating at the time of mineral carbonation.