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A framework for designing orthogonal chaotic phase-coded waveforms with space-time complementary coding (STCC) is proposed for multiple-input multiple-output (MIMO) radar applications. The phase-coded waveform set to be transmitted is generated with an arbitrary family size and an arbitrary code length by using chaotic sequences. Due to the properties of chaos, this chaotic waveform set has many advantages in performance, such as anti-interference and low probability of intercept. However, it cannot be directly exploited due to the high range sidelobes, mutual interferences, and Doppler intolerance. In order to widely implement it in practice, we optimize the chaotic phase-coded waveform set from two aspects. Firstly, the autocorrelation property of the waveform is improved by transmitting complementary chaotic phase-coded waveforms, and an adaptive clonal selection algorithm is utilized to optimize a pair of complementary chaotic phase-coded pulses. Secondly, the crosscorrelation among different waveforms is eliminated by implementing space-time coding into the complementary pulses. Moreover, to enhance the detection ability for moving targets in MIMO radars, a method of weighting different pulses by a null space vector is utilized at the receiver to compensate the interpulse Doppler phase shift and accumulate different pulses coherently. Simulation results demonstrate the efficiency of our proposed method.