A series of plate-impact experiments were conducted to investigate the influences of impact stress and microstructure on the shock and spall behaviors of a high specific strength steel (HSSS). The HSSS shows a strong positive strain rate sensitivity on the yield strength. With increasing impact stress up to about 6 GPa, the spall strength is found to decrease significantly and then levels off with further increasing impact stress. This trend is proposed to be attributed to the accumulation damage within the target as the initial shock-induced compression wave propagates through the target. The microcracks are clearly observed to nucleate from the interfaces between γ-austenite and B2 phase and propagate along the interfaces or cut through the B2 phase in the HSSS during the spalling process. The Hugoniot elastic limit and the spall strength were found to be highly dependent on the microstructure. The spall strength was found to be higher when the density of the void nucleation sites is lower, indicating that the spall strength should be a microstructure parameter of the HSSS under impact tensile conditions depending on the density of phase interfaces. It was also found that there is a tradeoff between the specific yield strength and the spall strength for this HSSS; thus, the current findings should provide insights for achieving an optimal combination of both mechanical properties for impact-resistant applications by tailoring the microstructure.