In the attitude maneuver scenarios of thin-film spacecraft intercepting non-cooperative targets，the attitude control is difficult due to the problems such as large area-mass ratio and large moment of inertia.In order to solve such problems，in this paper，an attitude maneuver control method based on a nonlinear variable structure sliding-mode controller is proposed.First，the flywheel is added to the common slider-sail mechanism of thin-film spacecraft as a cooperative control mechanism，and then an attitude control model is established with the consideration of the atmospheric disturbance torque，the flywheel friction torque，the inertia moment change，etc.Second，a nonlinear variable structure sliding mode controller is designed based on the error quaternion and the error angular velocity，and the stability of the control system is proved by the Lyapunov analysis method.Finally，a simulation experiment system of on-ground attitude adjustment for thin-film spacecraft based on the air-bearing platform is designed and built.The experimental results show that the controller proposed in this paper can realize the attitude maneuver control of the thin-film spacecraft in complex scenarios， restrains the influence of disturbance，and has some robustness.The work in this paper can provide an idea for the design of spacecraft controller with large area-mass ratio and large moment of inertia.