The equilibrium geometry and vibrational frequencies of tricyclo[3.1.0.0(2,6)]hexane have been determined at the MP26-311G(d,p) level by using ab initio calculations. An appropriate homodesmic reaction was used to determine the strain enthalpy and heat of formation, giving values of 71.3 and 57.3 kcal/mol, respectively. The strain energy and heat of formation are compared to those of structurally related molecules. The IR spectrum has been obtained in the gas phase and in an argon matrix, while the Raman spectrum was collected of the liquid sample. The vibrational fundamentals are assigned to specific normal modes by comparison of the calculated and experimental spectra.