Many examples of micro-and nanoscale particles made from atomic or molecular building blocks are known, with these systems having been extensively explored due to their useful properties. [1][2][3][4][5][6] Currently, efforts are ongoing to manipulate the composition, as well as its size and morphology, of particles as part of systematic attempts to alter their chemical and physical properties. Within this context, chemical transformation has emerged a useful method for tuning the composition. [ 7 , 8 ] Metal oxide materials have received a great deal of attention as a result of their functional properties that have made them of use in a wide range of fi elds including magnetics, [ 9 ] electronics, [ 10 ] optics, [ 11 ] catalysis, [ 12 ] and medical diagnostics. [ 13 ] ZnO and Co 3 O 4 , in particular, are attractive materials because they are a nonexpensive and nontoxic photoluminescent semiconductor and a magnetic p -type semiconductor, respectively. And they have many interesting applications in sensor, catalyst, electronic device, and solar cell. [10][11][12] Some hybrid metal oxide materials containing more than two metal composites within a particle have been described; these display modifi ed properties and have been proposed as candidates for multifunctional materials; [ 14 , 15 ] however, there is no general preparation method for hybrid metal oxide materials with tunable chemical compositions. Here we formulate a methodology that involves straightforward chemical transformation and continuous thermal treatment of the colloidal coordination polymer particles (CPPs) and show that it allows for the synthesis of composition-tunable multi ball-in-ball hybrid metal oxide particles through the cation exchange reaction. The work described here thus provides a way to access a variety of multicompositional hybrid metal oxides, something that should facilitate their eventual use in practical applications.Infi nite coordination polymers in which metal ions or metal clusters act as nodes to connect molecular building blocks consisting of organic or organometallic complexes have received many attention because of their useful applications such as gas storage, catalysis, optics, and separation. [ 16 ] Recently, the novel strategies for the synthesis of micro-and nano-sized particles made from infi nite coordination polymers, namely coordination polymer particles (CPPs), have been proposed and demonstrated. [ 2 , 8 , 17-20 ] Taking advantage of the unique reactivity and thermal behavior of CPPs, a number of spherical multi ball-in-ball hybrid metal oxides with tunable compositions have been logically formulated and prepared using the following straightforward processes; I) CPP preparation using a precipitation method, II) cation exchange reaction for composition transformation of CPPs, and III) a fi nal calcination processing of pre-prepared CPPs that engenders decomposition of the CPPs and formation of metal oxides ( Scheme 1 ). In general, the initial spherical CPPs, namely M-MSB-M ( 2 , M = Zn 2 + or Co 2 + , MS...