In this study, Fe-25Mn-xAl-8Ni-C alloys (x = 10 wt.%, 11 wt.%, 12 wt.%, 13 wt.%) were prepared by a vacuum arc melting method, and the microstructure of this series of alloys and the in situ tensile deformation behavior were studied. The results showed that Fe-25Mn-xAl-8Ni-C alloys mainly contained austenite phase with a small amount of NiAl compound. With the content of Al increasing, the amount of austenite decreased while the amount of NiAl compound increased. When the Al content increased to 12 wt.%, the interface between austenite and NiAl compound and austenitic internal started to precipitate k-carbide phase. In situ tensile results also showed that as the content of Al increased, the alloy elongation decreased gradually, and the tensile strength first increased and then decreased. When the Al content was up to 11 wt.%, the elongation and tensile strength were 2.6% and 702.5 MPa, respectively; the results of in situ tensile dynamic observations show that during the process of stretching, austenite deformed first, and crack initiation mainly occurred at the interface between austenite and NiAl compound, and propagated along the interface, resulting in fracture of the alloy.