A dual position-sensitive-detector (PSD)-based unit can be used for angular measurements of a multi-degree-of-freedom measurement system and a laser interferometry-based sensing and tracking system. In order to ensure the precision of incident beam direction measurement for a PSD-based unit, model and autoreflection alignment methods for correction of PSD-based unit parameters are proposed. Experimental results demonstrate the deviations between the angular measurements obtained using a dual PSD-based unit and an autocollimator varied by 70″, 20″, and 1″ for three runs of the autoreflection alignment method, respectively, and the model method deviations all varied by 1″ in the 1000″ measurement range for three runs. It is therefore concluded that the model method is more reliable than the autoreflection alignment method for ensuring the accuracy of a dual PSD-based unit.