Synergetic strengthening induced by plastic strain incompatibility at the interface, and the resulting extra geometrically necessary dislocations (GNDs) generated during plastic deformation, were investigated to understand the origin of extra strength in heterogeneous structured (HS) materials. The mechanism of extra GND generation in twinning-induced plasticity (TWIP)-interstitial free (IF) steel layered sheet was quantitatively analyzed by conducting in situ neutron scattering tensile test. Load partitioning due to the different mechanical properties between the TWIP-steel core and IF-steel sheath at the TWIP/IF interface was observed during the in situ tensile testing. Because of the plastic strain incompatibility from load partitioning, extra GNDs are generated and saturate during tensile deformation. The extra GNDs can be correlated with the back-stress evolution of the HS materials, which contributes to the strength of layered materials. Because of the back-stress evolution caused by load partitioning, the strength of TWIP-IF layered steel is higher than the strength estimated by the rule-of-mixtures. This finding offers a mechanism by which extra GNDs are generated during load partitioning and shows how they contribute to the mechanical properties of HS materials.