Nanostructured bainite was obtained in high-carbon Si-Al-rich steel by low-temperature (220–260 °C) isothermal transformation after austenitisation at different temperatures (900 °C, 1000 °C, and 1150 °C). Improved strength-ductility-toughness balance was achieved in the nanostructured bainitic steel austenitised at low temperatures (900 °C and 1000 °C). Increasing the austenitising temperature not only coarsened prior austenite grains and bainite packets, but also increased the size and fraction of blocky retained austenite. High austenitising temperature (1150 °C) remarkably decreased ductility and impact toughness, but had a small effect on strength and hardness.