In this study the geometry optimization of harmane using the semi-empirical (AM1, PM3, MNDO,) ab initio HF as well as the B3LYP method was performed. The calculated geometrical parameters of harmane were compared with the available crystallographic data to verify the extent to which theoretical models approximate the molecular structure of this compound. Additionally, some electronic properties of harmane in the neutral and monocationic form were calculated using various theoretical methods. The semi-empirical ZINDO-1 and TD/B3LYP calculations were carried out using the B3LYP/6-31+G(d,p) optimized geometry of harmane. The utility of the applied methods to predict properties of electronic transitions to the lowest excited singlet states of harmane was discussed.