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Three-variable chaotic synchronization has been implemented based on DNA chemical reaction networks (CRNs) in previous works. However, it is still difficult to realize the encryption and decryption of continuous signals. A scheme of secure communication is proposed based on chaotic coupling synchronization by DNA CRNs in this paper. Firstly, the CRNs of two three-variable chaotic systems are constructed using bimolecular representation. Secondly, according to the design principle of the coupling term and the theory of stability, the CRNs of the coupling term are designed to realize the synchronization of two chaotic systems. Finally, the oblique wave, square wave, and staircase wave signals are added into chaotic systems to realize encryption and decryption. The dynamic behavior of a three-variable chaotic system is verified by Visual DSD and MATLAB software. The synchronization proof and the experimental results of encryption and decryption are given. The results indicate that the proposed secure communication scheme is effective. This paper provides an application method for studying secure communication in the DNA field. [ABSTRACT FROM AUTHOR]