Herein, in addition to conventional b-CD-NSPs, the NSPs of a, g, HP-b, methyl-b, and SBE-b cyclodextrins were synthesized by a simple modified approach and thoroughly characterized. The control of CDs derivatization over structural dimensions and properties was clearly observed. It is interesting to note the complete transformation of b-CD from its crystalline form to its non-crystalline derivatives and the further reversal when the derivatives are prepared into NSPs including those of a and g-CDs (as observed by PXRD). The SEM images revealed the different morphologies and porous structure of NSPs and, in particular, the NSPs of methyl-b-CD exhibited regular spherical shapes. Two drugs of different categories, doxorubicin and captopril, were evaluated for loading efficiencies, which were found to significantly vary with cross-linker ratio (1 : 4 and 1 : 6) and CD types. Together, all the synthesized NSPs provide a new horizon to try to solve existing problems relating to drug delivery.