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While the majority of studies utilize commercial MB formulations, increasing experimental evidence indicates that distinct MB features critically determine their diagnostic and therapeutic performance. Here, it is shown that shell stiffness engineering of poly(alkyl cyanoacrylate) (PACA) MB, via introducing monomers with varying alkyl chain lengths and glass transition temperatures, preserves a narrow size distribution \u22482\u20133\u00a0\u00b5m, while enhancing MB drug loading, in vitro sonoporation capability, and in vitro and in vivo acoustic responses. All\u2010atom molecular dynamics simulations and spectroscopic experiments demonstrate that MB shell engineering increases drug diffusion rates in the shell, maximizing the loading capacity of the formulations. Atomic force microscopy demonstrates that the stiffness of the MB shell can be tailored by more than ten\u2010fold, boosting sonoporation and imaging performance. 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