The Sodium-Cooled Fast Reactor (SFR) is the most promising and technologically evolved among the six nuclear reactor concepts selected by the Generation IV International Forum. Although it is compatible with a closed fuel cycle for sustainable energy production, its competitiveness depends on being able to achieve high fuel burn-up up to 200 GWd/t. This would enable efficient fuel utilization to minimize fuel cycle costs. Hence, development of optimized core materials, especially for fuel cladding tubes that are subjected to extreme conditions of intense fast-spectrum neutron irradiation, high temperatures, and mechanical and chemical fuel–cladding interactions, continues to be a priority worldwide. Resistance to void swelling, irradiation creep, and embrittlement are required to be enhanced to minimize dimensional changes and loss of ductility in core components, which limit achievable burn-up. Current SFR core materials comprise austenitic stainless steels (SS) and ferritic-martensitic (FM) steels. Cold-worked austenitic SS grades 304, 316, 316Ti, niobium-stabilized grades FV548, EI-847, EP-172, and Ti-modified 15Cr-15Ni SS, such as D9, 1.4970, 15/15Ti SS, and ChS-68, have been used for fuel cladding and ducts in SFRs built to date, and they withstand neutron irradiation damage up to 80–100 dpa. Subsequent improvements have been made by optimizing minor elements (titanium, silicon, and phosphorous) and multi-stabilization to develop advanced grades such as Si-modified 15-15Ti, Indian Fast Reactor Advanced Clad (IFAC-1), PNC-316, EK-164, and HT-UPS, which could support burn-up of 150 GWd/t. In the case of FM steels, several commercial grades are found suitable in view of their inherent void swelling resistance to 200 dpa, and are being developed for improved creep strength by oxide dispersion strengthening to realize burn-up of 200–250 GWd/t. This article presents the development of structural materials for SFR fuel pin cladding and ducts and associated enhancement of permissible fuel burn-up. Indian and international experience resulting from extensive in-pile and out-of-pile mechanical testing and fuel–cladding interactions has been covered.