Homogeneous molecular catalysts and heterogeneous catalysts possess complementary strengths,and are of great importance in laboratory/commercial procedures.While various porous hosts,such as polymers,carbons,silica,metal oxides and zeolites,have been used in an attempt to heterogenize homogeneous catalysts,realizing the integration of both functions at the expense of discounting their respective advantages,it remains a significant challenge to truly combine their intrinsic strengths in a single catalyst without compromise.Here,we describe a general template-assisted approach to incorporating soluble molecular catalysts into the hollow porous capsule,which prevents their leaching due to the absence of large intergranular space.In the resultant yolk (soluble)-shell (crystalline) capsules,the soluble yolks can perform their intrinsic activity in a mimetic homogeneous environment,and the crystalline porous shells endow the former with selective permeability,substrate enrichment,size-selective and heterogeneous cascade catalysis,beyond the integration of the respective advantages of homogeneous and heterogeneous catalysts.