High borated stainless steel sheets have been widely applied in the nuclear power industry because of good thermal neutron absorption property. However, the large and network-like borides existing around the austenite grains in the conventional ingot casting steel seriously deteriorate the hot workability and the mechanical properties at ambient temperature. In this work, we tried to acquire ultra-fine microstructure by sub-rapid solidification using a novel twin-roll strip casting technology so as to enhance the mechanical properties of 2.1%B austenitic stainless steel. Surprisingly, dispersive and very fine borides mostly smaller than 5 µm were produced in the as-cast microstructure without network-like distribution. The morphologies and crystal structure of borides as well as the stacking faults in borides were investigated in detail. After subsequent hot-rolling and solution treatment, ultra-fine borides were observed with more than 50% of which in a size range of 0.3–1.5 µm, significantly smaller than those of the conventional ingot casted and hot rolled steel. Benefiting from the ultra-fine borides, excellent mechanical properties which had not been reported were obtained. In particular, a total elongation of 14.1% was exhibited, which was twice as high as that of the conventional ingot casted and hot rolled steel. Thus a new structure-function combining high borated stainless steel sheet was achieved. The strengthening and plasticity increasing mechanism was discussed based on Hall-Petch relationship, Orowan mechanism and strain-hardening rate analysis. The fracture behavior in tensile deformation was studied in detail. A characteristic fracture process accompanied with the initiation and coalescence of cavities in austenite matrix was found. This work not only developed a new processing way to produce high borated stainless steel with excellent mechanical properties, but also provided a potential solution for some other hard-worked metallic materials with brittle eutectic phase.