The invention discloses an attitude control system and a control method of a four-rotor aircraft. Firstly, the information of attitude angles of the current aircraft is obtained, and the attitude angles include a roll angle, a pitch angle and a yaw angle; secondly, controllers for the roll angle, the pitch angle and the yaw angle are respectively designed, wherein the controller for the roll angle is the same as that for the pitch angle; and finally, after obtained control inputs of the three controllers are overlapped, a total driving signal is output, thereby driving a motor to operate, so as to control the attitude of the aircraft. A gyroscope and an accelerometer are combined, and a Kalman filter is designed in accordance with models of the attitude angles of the aircraft, so as to conjecture the attitude angles on line. Additionally, variables of the intermediate state of the system can be obtained, and a certain filtering effect is achieved.