Nanostructured powder particles of Fe3Al and (Fe,Ti)3Al phases were produced using mechanical alloying. These intermetallic phases with a nearly complete density were consolidated by spark plasma sintering. The mechanical properties of the bulk samples, i.e., elasticity modulus, hardness, and plasticity index, and also their tribological behavior were investigated using nanoindentation and nano-scratch tests. It was found that both Fe3Al and (Fe,Ti)3Al phases can be synthesized after 30 h of high-energy ball milling. In addition, no phase evolution was observed after spark plasma sintering. An analysis of the atomic force microscope images obtained from the nanoindentation tests showed a higher elasticity modulus, higher hardness, and lower plasticity index due to the addition of Ti to the Fe3Al system. (Fe,Ti)3Al displayed better tribological properties as compared with Fe3Al. A smaller volume of the scratched line was clearly seen in the atomic force microscope images of the nanostructured (Fe,Ti)3Al compound.