High-quality LDH-SO4-CO3 whiskers were synthesized via liquid precipitation method using MgSO4·7H2O and Al2(SO4)3·18H2O as precursors and Na2CO3-NaHCO3 buffer solution as precipitant. The influence of buffer solution concentration on the characteristics of the samples was investigated. The as-grown whiskers were characterized by X-ray diffraction, transmission electron microscopy, and Brunauer-Emmett-Teller N2 specific surface area measurements. The results show that the buffer solution concentration has significant impact on whiskers with intercalated structure. The LDH-SO4-CO3 whiskers with well-defined geometry, distinct intercalated structure, decent quality, and excellent dispersing capability can be obtained under the following conditions: buffer solution volume ratio of 45%, reaction temperature of 83°C, and reaction time of 182 h. The obtained whiskers are well-crystallized and exhibit homogeneous morphology consisting of fber bars.