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The mechanical properties and failure behavior of single tire belts with different cord angles were investigated. The cords consisted of two pairs of twisted steel wires. Geometric moiré and the grid method were used to measure small and large deformations, respectively. The stress–strain curves of all samples tested display three typical deformation stages, initial nonlinear deformation, followed by an intermediate stage of approximately linear deformation and a final stage of approximately linear deformation with increased modulus. The transition strain from the first to the second stage increases linearly with cord angle and the ultimate strength is found to follow the Tsai–Hill failure criterion. Failure mechanisms varied with cord angle. They are classified into four modes including failure within the cord, shear failure at the interface between cord and rubber, a combination of the above two modes and cord breakage. In-plane shear properties were obtained using both the Arcan pure shear and the 22° off-axis tests. They were found to be in good agreement. A nonlinear micromechanics model was proposed to predict the properties of single belts with different cord orientations by taking into consideration both the material and geometric nonlinearities.