Dedicated to Dr. Manfred Flad on the occasion of his 90th birthdayPreparing a material that has particles of uniform dimension has been one of the biggest challenges for chemists as well as material scientists. The traditional ways of imparting order at the nanoscopic level have changed since the synthesis of fullerene clusters.[1] The use of techniques such as epitaxy and metal-organic chemical vapor deposition (MOCVD) have been used extensively in this regard. The synthesis of giant inorganic molecules, such as polyoxoanions, [2] Al 77 , [3] and Ga 84 [4] clusters are examples of inorganic counterparts of fullerenes. The synthesis of metal phosphonates using organometallic routes in recent years has led to the realization of a series of oligomeric transition-metal and main-group-metal phosphonates. [5, 6] In all these reports, the size of the oligomeric structure is highly dependent on the substituent on the metal center as well as at the phosphorus center. The metal phosphonates can be synthesized either using metal precursor-phosphonic acid interactions via an acid exchange or by starting from metal alkyls/amides/alcoholates by elimination of alkanes/amines/alcohols. [5][6][7] It has been demonstrated that metals belonging to the same group of the periodic table yield molecular phosphonates of the same topology if the substituents on the metal and phosphorus centers are kept the same. Although examples of zinc phosphonates following both the synthetic methodologies have been reported, there have been no examples of molecular cadmium phospho-