Atmospheric drag is an important factor affecting orbit determination and prediction of low-orbit space debris. To obtain accurate ballistic coefficients of space debris, we propose a calculation method based on measured optical angles. Angle measurements of space debris with a perigee height below 1400 km acquired from a photoelectric array were used for orbit determination. Perturbation equations of atmospheric drag were used to calculate the semi-major-axis variation. The ballistic coefficients of space debris were estimated and compared with those published by the North American Aerospace Defense Command in terms of orbit prediction error. The 48 h orbit prediction error of the ballistic coefficients obtained from the proposed method is reduced by 18.65% compared with the published error. Hence, our method seems suitable for calculating space debris ballistic coefficients and supporting related practical applications.