Security is one of the key issues in communications, but it has not attracted much attention in the field of underwater wireless optical communication (UWOC). This Letter proposes a UWOC encryption scheme with orthogonal frequency division multiplexing (OFDM) modulation, based on the three-layer chaotic encryption and chaotic discrete Fourier transform (DFT) precoding. The three-layer chaotic encryption processes are bit stream diffusion, in-phase/quadrature encryption, and time-frequency scrambling. With multi-fold data encryption, the scheme can create a keyspace of 9.7×10179, effectively resisting brute force attacks and chosen-plaintext attacks. A 3 Gbit/s encrypted OFDM signal is successfully transmitted over a 7 m water channel.