Metal-organic frameworks (MOFs)-based yolkshell nanostructures have drawn enormous attention recently due to their multifunctionality.However,the regulations of the sizea nd morphology of yolk-shell nanostructures are still limited by the unclear formation mechanism. Herein, we first demonstrated as olvent-dependent adsorption-driven mechanism for synthesizing yolk-shelled MOFs-based nanostructures coated with mesoporous SiO 2 shells (ZIF-8@mSiO 2)with tunable sizea nd morphology.T he selective and competitive adsorption of methanol (CH 3 OH) and water (H 2 O) on ZIF-8 core were found to have decisive effects on inducing the morphology evolution of yolk-shell nanostructures.T he obtained yolk-shelled ZIF-8@mSiO 2 nanostructures show great promise in generating acoustic cavitation effect for sonodynamic cancer therapyi nvitro.W eb elieve that this work will not only help us to design novel MOFs-based yolkshell nanostructures,b ut also promote the widespread application of MOFs materials.