Iron-induced self-assembly of beta-cyclodextrin, beta-CD, into size controllable nanospheres with a well-defined spherical morphology and a relatively narrow size distribution wits formed when acetone was added to it solution of beta-CD with iron(II) acetate, Fe(OAc)(2), in DMF. Thermogravimetric analysis, inductively coupled plasma atomic emission spectroscopy, and high resolution transmission electron microscopy showed that the irons were present as it well-dispersed state in the beta-CD nanospheres. In the H-1 NMR Spectrum of the beta-CD/Fe(OAc)(2), beta/Fe, solution before adding acetone, the peaks corresponding to beta-CD were broadened and their spin-spin splitting had disappeared. In particular the beta/Fe solutions were found to remain in a clean solution state at 1 week after Solution preparation. These findings indicate the isolation of individual iron ions caused by the surrounding of each ion with the beta-CD molecules in the solution before the addition of acetone. X-ray crystal structure analysis, morphological observations, and N-2 adsorption and desorption experiments showed that the beta-CD nanospheres were generated by the formation of iron-embedded beta-CD primary particles with disordered cage type structure and simultaneous spherical assembly of the primary particles during the addition of acetone to the beta/Fe solution with appropriate mole ratio between beta-CD and Fe(OAc)(2). Interestingly, the size of the beta-CD nanospheres could be simply controlled by changing the speed at which acetone was added to the Solution, with higher acetone addition speeds yielding smaller particles.