Strontium sulfate (SrSO4) sisal-like hierarchical structures (SLHS) were successfully synthesized by using SrCrO4nanowires in mother solution as precursor to react with Na2SO4 aqueous solution at room temperature. The SrSO4 SLHS have a uniform diameter of about 6 μm, which are composed of single-crystalline SrSO4 nanopyramids oriented radially to their centre. The nanopyramids, which grow along [010] direction, are about 300–500 nm and 20–50 nm for the roots and tips in diameter and 1–3 μm in length. The controlled experimental results indicate that the formation mechanism of the SrSO4 SLHS is related to the “two-step” growth process.