Inconclusive findings regarding the collagen fiber architecture and the material properties of the glenohumeral capsule make it unclear whether the material symmetry of the glenohumeral capsule is isotropic or anisotropic. The overall objective of this work was to use a combined experimental and computational protocol to characterize the mechanical properties of the axillary pouch of the glenohumeral capsule and to determine the appropriate material symmetry. Two perpendicular tensile and finite simple shear deformations were applied to a series of tissue samples from the axillary pouch of the glenohumeral capsule. An inverse finite element optimization routine was then used to determine the material coefficients for an isotropic hyperelastic constitutive model by simulating the experimental conditions. There were no significant differences between the material coefficients obtained from the two perpendicular tensile deformations or finite simple shear deformations. Furthermore, stress-stretch relationships predicted by utilizing the material coefficients from one direction were able to predict the responses of the same tissue sample in the perpendicular direction. These similarities between the longitudinal and transverse material behaviors of the tissue imply that the capsule may be considered an isotropic material. However, differences did exist between the material coefficients obtained from the tensile and shear loading conditions. Therefore, a more advanced constitutive model is needed to predict both the tensile and shear responses of the material.