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In this study, a double-walled and pomelo-like hierarchical shear thickening fluid (STF) is successfully encapsulated using the simple and environment-friendly calcium alginate encapsulation technique by instilling STF into sodium alginate (SA) and crosslinking by calcium chloride solution. The encapsulated STF has a pomelo-like structure with a shell thickness of 2.9 μm and core pores with a size of 21.43 μm. The effect of the size of STF capsules (2.10, 1.89, 1.86, 1.83, 1.73, and 1.63 mm) is explored in terms of thermal stability, swelling capacity, mechanical property, and release performance. The buffering performance of different sizes of STF-containing capsules is also investigated. The pomelo-like STF capsules can withstand a processing temperature of 250 °C. With a decrease in particle size, the compression strain energy slowly increases first and then rapidly enhances. The kinetic release of pomelo-like STF capsules conforms to Fickian diffusion. STF-containing capsules with a diameter of 1.83 mm present the greatest thermal stability, the highest STF amount, the maximum swelling coefficient, and the fastest kinetic diffusion. STF-containing capsules also have an improved buffering performance in PU foam. This capsule has the best comprehensive performance and can adapt to diversified applications, such as personnel armor and other protective sports equipment.
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