Advanced intermetallic TiAl alloys have attracted considerable attention as a high-temperature structural material in aerospace and automobile sectors owing to their low density, elevated temperature strength, superior creep, and oxidation resistance. The present study is focused on assessing the effect of alloy composition, heat treatment and microstructural variation on the bulk and small-scale deformation behavior of commercial grade 2nd generation and newly developed 3rd generation TiAl alloys at 25 °C (298 K), 300 °C (573 K), and 500 °C (773 K). Twinning is noted to be the dominant deformation mechanism irrespective of the temperature. The highest yield strength and hardness are noted for the as-cast 3rd generation TiAl alloy owing to the finer microstructure and compositional variation. Heat treatment however modifies the TiAl microstructure significantly resulting to unique bilamellar-biglobular (BLBG) microstructure, devoid of the brittle β0 phase. Consequently, nano twins- and micro twins-induced enhanced deformability is noted for such microstructure, as compared to the as-cast counterparts. Interestingly, an anomalous increase in strength with an increase in temperature is observed for the studied alloys owing to the presence of high-density twins and Kear-Wilsdorf locks. Most importantly, a temperature dependant hardness anomaly is noted in the TiAl alloys that opens new avenues for further research in nanoscale deformation. This piece of research potentially strengthens the understanding of the role of constituent phases and temperature in the deformation behavior of complex TiAl alloys. Twin-induced deformation mechanism noted for the novel BLBG microstructure, can also be valid for different generations of TiAl alloys to achieve enhanced deformability that paves the way for the development of next-generation material.