Existing 64-QAM Golay complementary pairs, each having impulse-like aperiodic auto-correlation sums, have been used to generate codebooks in code-keying orthogonal frequencydivision multiplexing (OFDM) communications for the peak-tomean power control. As a generalization of the 64-QAM Golay complementary pairs, in this paper, 64-QAM complementary sets, each of which contains two or more sequences, are proposed. It is shown that when the set size is not less than 4, they lead to significant code rate increases in code-keying OFDM communications.