In this article, a complementary sliding mode (CSM) controller using a self-constructing Chebyshev fuzzy recurrent neural network (SCCFRNN) is proposed for harmonic suppression control of an active power filter (APF). The SCCFRNN whose structure can be automatically learned through the designed structure self-learning algorithm is introduced to approximate the unknown nonlinear term in the APF dynamic model, so as to improve modeling accuracy and reduce the burden of CSM control (CSMC). The SCCFRNN combines the advantages of a fuzzy neural network (FNN), recurrent neural network (RNN), and Chebyshev neural network (CNN), and all parameters can be adjusted according to the designed adaptive laws. Eventually, through detailed simulation, hardware experiments, and fair comparison, the feasibility and superiority of the proposed control algorithm were verified.