In this work, a simple, fast, and green method for synthesis of hierarchical SrCO3 architectures without outside additives was successfully developed on the basis of the strategy of CO2 capture, utilization and storage, in which the 1,4‐butanediol‐based CO2‐storage material (BDO‐based CO2SM) and Sr(OH)2 solution were used as the reaction reagents. The BDO‐based CO2SM, which derived from the CO2 fixation with the system of 1,4‐butanediol (BDO) + 1,2‐ethanediamine (EDA), was utilized as both a CO2 source and a crystal modifier to regulate and control the nucleation, crystallization, and growth of SrCO3 crystals. Meanwhile, a systematic study of the influence of significant experimental parameters, including BDO‐based CO2SM concentration, reaction temperature, and reaction time, on the morphology and size of SrCO3 crystals was carried out. And the synthesized products were indexed to the pure orthorhombic phase of strontianite via XRD patterns and FTIR spectra. Moreover, after the precipitation of SrCO3 crystals in 120 g⋅L−1 BDO‐based CO2SM solution, the filtered solution could not only be reused to absorb CO2, but also to prepare the same crystal phase SrCO3 repeatedly with the addition of Sr(OH)2.