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A new differential space-time code, called differential space-time block-diagonal code (DSTBDC), is proposed for multiple-input multiple-output (MIMO) wireless communication systems. By exploiting the block-diagonal construction of DSTBDC, we can design a variety of high-performance DSTBDC, especially for the cases of large numbers of transmit antennas and high date rates. In flat fading channels, DSTBDC outperforms traditional differential space-time codes if the data rate is higher than 1 bps/Hz, especially when the number of transmit antennas is large. In frequency-selective fading channels, multiple-input multiple-output orthogonal frequency-division multiplexing (MIMO-OFDM) systems using DSTBDC have the powerful ability to achieve very high diversity gain in space, time, and frequency simultaneously. Due to the special orthogonal construction, DSTBDC has a simple decoding algorithm. In addition, DSTBDC can significantly save the cost of radio frequency circuits.