Autocollimators (ACs) are primarily used for two-dimension measurement with small angle. A three-dimensional AC (3D-AC) with a large measurement range and capable of 3D angle measurement is proposed based on a modified cube corner reflector (MCCR). The MCCR structure is designed by establishing the space coordinate vector relation model between AC and the reflectors with the rotation relation of Euler space. A 3D-AC angle measurement equation for MCCR dimension angle recognition is established. Experiments demonstrate that the proposed 3D-AC model can be used for 3D measurement. The measurement range of 3D-AC is 10°, and the uncertainty values for the one-dimensional and combined angle measurements are (57.10″, 55.25″, 40.43″) and (394.16″, 455.36″, 319.57″), respectively.