In this paper,w eh ave established as imple and generalizable sprout-like growth method for the facile synthesis of Janus mesoporous silica nanostructures with organic-inorganich ybrid components by using periodic mesoporous organosilica (PMO)n anoparticles as seeds with mesoporous SiO 2 as branches growing on the PMO surface. The morphology of Janus nanostructures with different lengths and numbers of SiO 2 branches can be easily controlled by varying the tetraethoxysilane concentration in the synthesis system.T he Janus nanostructures are also easily modified with different SO 3 Ha nd NH 2 groups on the SiO 2 branches and PMO cores, respectively,and exhibit excellent catalytic performance in the deacetalizationHenry cascade reaction.Recently,J anus nanostructures have emerged as an ew family of colloidal structured materials, [1] and attracted the attention of many researchers owing to their potential applicationsi n many fields such as drug delivery, [2] imagingp robes, [3] electronic devices, [4] andc atalysis. [5] Janus nanostructures have many advantages compared with other complex nanoparticles, [6] such as combing individual components together, [6a] even incompatible acidic and basic groups, and retaining their intrinsic properties.[6d] Now,m any methods for preparing Janus nanostructures have been reported, including one-step synthesis, [7] surface chemical-selective modification, [8] self-assembly, [9] and others.[10] Althoughm any effortsh aveb een made to fabricate Janus nanostructures, [1] the effective methods for synthesis of Janus nanostructures are still limited, [6c, 11] and the prepared Janus nanoparticles are typically singlecomponent.Mesoporouss ilica nanomaterials have received considerable attention because of their potential applications in catalysis, separation, drug delivery,a nd so forth, and mesoporous silica nanomaterials have many advantages over solid materials including large surface area and pore volume, stability,a nd the option to functionalize their outer or inner surfaces.[12] Av ariety of mesoporous silica nanomaterials have been successfully synthesized, including SBA-15t ype nanoparticles, [12a] MCM-41 type nanoparticles, [13] core-shell [12c] or yolk-shell [14] structured mesoporouss ilica nanospheres, and periodic mesoporous organosilica (PMO)n anoparticles.[15] However,t he traditional synthesis methods form esoporous silica nanomaterials often rely on one-pot sol-gelp rocesses or template methods, [12b, 15] and most products of these methods are analogous sphereso r single-component materials. The organic and inorganic hybrid nanomaterials based on mesoporouss ilica have many advantages over the traditional single-component nanomaterials, including good stability,t ailoreds urfacep olarities, and even good biocompatibility for different applications.[16] Thus, it remains ag reat challenge to develop af acile and scalable approach for preparing Janus mesoporouss ilica nanostructures with organic-inorganic hybrid components.Herein, we developasimpl...