Isomers of the higher fullerenes were analyzed using 3He NMR spectroscopy. Structures have been assigned to isomers for C76, C78 and C84. Several fullerene hydrides, C60H n (n = 2, 4, 6, 8, 18, 36), have been synthesized using a novel hydrazine reduction. Other fullerene hydrides, C60Hn (n = 38, 40, 42, 48), were synthesized via the Birch reduction of the hydrazine reduction products. Seven of eight isomers for C60H4 have been observed in the proton NMR spectra. 3He NMR spectra were obtained for 3He C60H4, 3He C 60H18 and 3He C60H36. These spectra revealed six isomers for C60H4, one isomer for C60H18 and two isomers for C60H 36. The most intense signal in the 3He spectrum for C 60H36 was assigned to the isomer of D3d' symmetry based on the 3He NMR chemical shift value. High field proton NMR analyses (750 MHz) of C60H2 and C60H4 in 1:1 solutions of CS2:C 6D6 gave spectra with signals which showed unexpected additional fine structure as a result of an alignment effect caused by the orientation of benzene in a strong magnetic field.