Comparing to orthogonal localized molecular orbitals (OLMO), the nonorthogonal localized molecular orbitals (NOLMO) exhibit bonding pictures more accordant with those in the traditional chemistry. They are more contracted, so that they have a better transferability and better performances for the calculation of election correlation energies and for the linear scaling algorithms of large systems. The satisfactory NOLMOs should be as contracted as possible while their shapes and spatial distribution keep in accordance with the traditional chemical bonding picture. It is found that the spread of NOLMOs is a monotonic decreasing function of their orthogonality, and it may reduce to any extent as the orthogonality descends. However, when the orthogonality descends to some point, the shapes and spatial distribution of the NOLMOs deviate drastically from the traditional chemical bonding picture, and finally the NOLMOs tend to linear dependence. Without the requirement of orthogonalization, some other constrain Comparing to orthogonal localized molecular orbitals (OLMO), the nonorthogonal localized molecular orbitals (NOLMO) exhibit bonding pictures more accordant with those in the traditional chemistry. They are more contracted, so that they have a better transferability and better performances for the calculation of election correlation energies and for the linear scaling algorithms of large systems. The satisfactory NOLMOs should be as contracted as possible while their shapes and spatial distribution keep in accordance with the traditional chemical bonding picture. It is found that the spread of NOLMOs is a monotonic decreasing function of their orthogonality, and it may reduce to any extent as the orthogonality descends. However, when the orthogonality descends to some point, the shapes and spatial distribution of the NOLMOs deviate drastically from the traditional chemical bonding picture, and finally the NOLMOs tend to linear Without the requirement of orthogonalization, so me other constrain