A low-carbon micro-alloyed (LCMA) steel with a body-centered cubic (bcc) crystal structure suitable for extremely low temperatures was developed by overcoming the intrinsic ductile-to-brittle transition in bcc alloys at cryogenic temperatures. The excellent cryogenic-to-ambient impact toughness in the LCMA rolled plate results from its heterogeneous microstructure, which gradually changes from bamboo-like ultrafine grains (∼ 1.1 μm) on the surface to relatively equiaxed coarse grains in the core (∼ 3.4 μm), accompanied by a distinct texture gradient variation. The heterostructured LCMA steel displays a cryogenic impact toughness of ∼200 J/cm2 at 77 K, which is 24 times higher than the coarse-grained LCMA steel. Such high impact toughness of heterostructured LCMA arises from the coordinated deformation mechanisms over different length-scales coupled with delamination toughening. At 77 K, the heterostructured steel plate deforms by forming cellular sub-structures at the core to the surface, which refines the microstructure and promotes hetero-deformation induced (HDI) hardening to improve intrinsic toughening. Moreover, the subsequent delamination process induces extrinsic toughening by shielding and blunting the cracks, with the local plane-stress conditions induced by delamination promoting ductile fracture of the coarse grains in the core regions. This low alloy steel with its heterogeneous microstructure exhibits extraordinary impact toughness at cryogenic temperatures highlights the possibility of materials design strategies for sustainable development.