This paper shows a method to design complementary filter using least square. The complementary filter is one of useful filters estimating angle. The basic concept of this filter is to enhance advantages of each sensor that angle detecting using a gyroscope has good accuracy at a high frequency and an accelerometer at a low frequency. When designing complementary filter, the most commonly used method is using cut-off frequency. However, it may be not easy to obtain a cut-off frequency. This paper presents a systematic method to determine the coefficients of the complementary filter using well-known linear least squares minimizing error between estimating angle and true angle.