Isomers of C60H36 and He@C60H36 have been synthesized by the Birch or dihydroanthracene reduction of C-60 and isolated by preparative high-pressure liquid chromatography. He-3, C-13, and IH NMR spectroscopic properties were then determined. A comparison of experimental chemical shifts against those computed using density functional theory (B3LYP) with polarized triple- and double-zeta basis sets for lie and C,H, respectively, allowed provisional assignment of structure for several isomers to be made. Theoretical calculations have also been carried out to identify low-energy structures. The transfer hydrogenation method using dihydroanthracene gives a major C60H36 isomer and a minor C60H36 isomer with C-3 symmetry as determined by the C-13 NMR Spectrum of C60H36 and the He-3 NMR spectrum of the corresponding sample of He-3@C60H36. In view of the HPLC retention times and the He-3 chemical shifts observed for the Birch and dihydroanthracene reduction products, the two isomers generated by the latter procedure can be only minor isomers of the Birch reduction. A significant energy barrier apparently exists in the dihydroanthracene reduction of C-60 for the conversion of the C-3 and C-1 symmetry isomers of C60H36 to the T symmetry isomer previously predicted by many calculations to be among the most stable C60H36 isomers. Many of the H-1 NMR signals exhibited by C60H36 (and C60H18, previously reported) are unusually deshielded compared to "ordinary" organic compounds, presumably because the unusual structures of C60H36 and C60H18 result in chemical shift tensors with one or more unusual principal values. Calculations clearly show a relationship between exceptionally deshielded protons beta to a benzene ring in C60H18 and C60H36 and relatively long C-C bonds associated with these protons. The additional information obtained from 1D and 2D H-1 NMR spectra obtained at ultrahigh field strengths (up to 900 MHz) will serve as a critical test of chemical shifts to be obtained from future calculations on different C60H36 isomers.