In this work, we briefly report some attempts to control regioisomeric bisadditions on Sc3N@I-h-C-80 and Lu3N@I-h-C-80 using the tether-controlled multifunctionalization method. We then describe the use of independent (nontethered) bis-1,3-dipolar cycloaddition reactions and the characterization of 5 new bisadducts, 3 for Sc3N@C-80 and 2 for Lu3N@C-80, which have never been reported before. Unexpectedly and remarkably, 4 of these compounds exhibit relatively high symmetry and 2 of these bisadducts are the first examples of intrinsically chiral endohedral compounds, due to the addition pattern, not to the presence of chiral centers on the addends. Since an analysis of the statistically possible number of bisadduct isomers on an I-h-C-80 cage has not been reported, we present it here.