The auracarboranes 1,2-(2) have been synthesized. Both compounds were characterized by NMR and X-ray crystallography. Compound 2 was found to contain an aurophilic interaction between the gold centers. A variable-temperature NMR investigation indicated that the energy barrier separating the gold-gold bonded state and the nonbonded state is 11 ( 1 kcal/mol. Compound 1 crystallized in the monoclinic space group P2 1 /c with a ) 18.3380(9) Å, b ) 14.1037(6) Å, c ) 19.4716(8) Å, ) 112.003(2)°, V ) 4669 Å 3 , and Z ) 4. Data were collected using Mo KR radiation, to a maximum 2θ ) 50°, giving 8865 unique reflections, and the structure was solved by heavy atom methods. The final discrepancy index was R ) 0.047, R w ) 0.055 for 3423 independent reflections with I > 3σ(I). Compound 2 crystallized in the monoclinic space group P2 1 /c with a ) 14.058(6) Å, b ) 18.365(8) Å, c ) 20.387(9) Å, ) 109.22(1)°, V ) 4970 Å 3 , and Z ) 4. Data were collected using Mo KR radiation, to a maximum 2θ ) 45°, giving 5232 unique reflections, and the structure was solved by heavy atom methods. The final discrepancy index was R ) 0.066, R w ) 0.069 for 2536 independent reflections with I > 3σ(I).