Compared with conventional optical elements, free-form surface optical elements, as a kind of nonrotationally symmetrical shaped component, can provide more freedom in optical design, optimize the structure of the optical system, and improve its performance. However, the difficulties involved in the measurement of free-form elements restrict their manufacture and application. A tilted-wave-interferometer (TWI) can achieve high precision in free-form surface measurement, but it requires higher space attitude error control. We analyze the relation between the alignment error and the measurement error introduced by the misalignment in free-form surface metrology with TWI. The attitude control method in the rotation direction is proposed based on the moire fringe technique. Then, combining it with the five-dimensional space attitude control method of aspherical elements, we put forward an alignment error control process in measuring the free-form surface. An experiment of measuring a free-form surface using TWI shows the effectiveness of our method.