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A novel preamble sequence design for random access using complete complementary code sets in multi-input multi-output orthogonal frequency division multiplexing (MIMO-OFDM) scheme is proposed. By elaborate design, both the optimum cross-correlation function (CCF) property and sufficient available number of preamble sequences can be achieved. The generation method and the bound of extension code number are addressed to satisfy the requirement of practical system. In addition, the comparison between proposed code and constant amplitude zero auto-correlation (CAZAC) code which is promising in the long term evolution of 3rd generation systems as preamble sequences was presented. The numerical results show that the application of preamble sequences with complete complementary code sets can obtain high detection probability.