The fabrication deviation of prisms and the error crosstalk are two major factors that produce serious systematic errors in dual-beam roll measurement based on a rhombic prism, and an error compensation method is put forward in this letter to reduce these systematic errors. The rotation matrix, reflection matrix, and refraction matrix are used to calculate and obtain the mathematical relationship model of the roll angle as well as the fabrication deviation of prism and error crosstalk. The fabrication deviation can be obtained through comparison experiments and using the least square method. In this way, the systematic error of the roll measurement caused by fabrication deviation of prism and error crosstalk can be eliminated theoretically. The experimental results show that the maximum error of the roll angle measurement reduces evidently to 3.5′′ from the previous 347.2′′ after compensation.