Severe plastic deformation (SPD) is effective in producing bulk ultrafine-grained and nanostructured materials with large densities of lattice defects. This field, also known as NanoSPD, experienced a significant progress within the past two decades. Beside classic SPD methods such as high-pressure torsion, equal-channel angular pressing, accumulative roll-bonding, twist extrusion, and multi-directional forging, various continuous techniques were introduced to produce upscaled samples. Moreover, numerous alloys, glasses, semiconductors, ceramics, polymers, and their composites were processed. The SPD methods were used to synthesize new materials or to stabilize metastable phases with advanced mechanical and functional properties. High strength combined with high ductility, low/room-temperature superplasticity, creep resistance, hydrogen storage, photocatalytic hydrogen production, photocatalytic CO₂ conversion, superconductivity, thermoelectric performance, radiation resistance, corrosion resistance, and biocompatibility are some highlighted properties of SPD-processed materials. This article reviews recent advances in the NanoSPD field and provides a brief history regarding its progress from the ancient times to modernity. Abbreviations: ARB: Accumulative Roll-Bonding; BCC: Body-Centered Cubic; DAC: Diamond Anvil Cell; EBSD: Electron Backscatter Diffraction; ECAP: Equal-Channel Angular Pressing (Extrusion); FCC: Face-Centered Cubic; FEM: Finite Element Method; FSP: Friction Stir Processing; HCP: Hexagonal Close-Packed; HPT: High-Pressure Torsion; HPTT: High-Pressure Tube Twisting; MDF: Multi-Directional (-Axial) Forging; NanoSPD: Nanomaterials by Severe Plastic Deformation; SDAC: Shear (Rotational) Diamond Anvil Cell; SEM: Scanning Electron Microscopy; SMAT: Surface Mechanical Attrition Treatment; SPD: Severe Plastic Deformation; TE: Twist Extrusion; TEM: Transmission Electron Microscopy; UFG: Ultrafine Grained GRAPHICAL ABSTRACT IMPACT STATEMENT This article comprehensively reviews recent advances on development of ultrafine-grained and nanostructured materials by severe plastic deformation and provides a brief history regarding the progress of this field.

Metal oxynitrides are promising photocatalysts due to their narrow bandgap, but their lower stability compared to metal oxides is a drawback. The introduction of high-entropy alloys with entropy-stabilization features has shown high potential for various functional applications in recent years. By considering these two types of materials, we developed a high-entropy oxynitride for photocatalytic water splitting. The material, with a general composition of TiZrHfNbTaO₆N₃ and a d⁰ electronic configuration, showed a narrow bandgap of 1.6 eV, which is much lower than the bandgaps of relevant binary and high-entropy oxides. The material exhibited photocurrent generation and photocatalytic hydrogen production with high chemical stability, suggesting the high potential of high-entropy oxynitrides as advanced low-bandgap and stable photocatalysts.