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The parallel spindle heads with high rotational capability are demanded in the area of multi-axis machine tools and 3D printers. This paper focuses on designing a class of 2R1T (R: Rotation; T: Translation) parallel spindle heads and the corresponding collaborative 5-axis manipulators with 2-dimension (2D) large rotational angles. In order to construct 2D rotational degrees of freedom (DOFs), a platform with 2D revolute joints is proposed first. Based on the constraint screw theory, the feasible limbs that can be connected in the platform are synthesized. In order to provide constant rotational axis for the platform, a class of redundant limbs are designed. A class of redundant 2R1T parallel spindle heads is obtained by connecting the redundant limbs with the platform and the redundant characteristics are verified by the modified Grübler-Kutzbach criterion. The corresponding 5-axis collaborative manipulators are presented by constructing a 2-DOF series translational bottom moving platform. The inverse kinematics and the orientation workspace as well as the decoupling characteristics of this type of 2R1T parallel spindle heads are analyzed. The results show that these manipulators have large 2D rotational angles than the traditional A3/Z3 heads and can be potentially used in the application of multi-axis machine tools and the 3D printers.