Ordered mesoporous carbons (OMCs) have demonstrated great potential in catalysis, and as supercapacitors and adsorbents. Since the introduction of the organic–organic self-assembly approach in 2004/2005 until now, the direct synthesis of OMCs is still limited to the wet processing of phenol-formaldehyde polycondensation, which involves soluble toxic precursors, and acid or alkali catalysts, and requires multiple synthesis steps, thus restricting the widespread application of OMCs. Herein, we report a simple, general, scalable and sustainable solid-state synthesis of OMCs and nickel OMCs with uniform and tunable mesopores (∼4–10 nm), large pore volumes (up to 0.96 cm³ g⁻¹) and high-surface areas exceeding 1,000 m² g⁻¹, based on a mechanochemical assembly between polyphenol-metal complexes and triblock co-polymers. Nickel nanoparticles (∼5.40 nm) confined in the cylindrical nanochannels show great thermal stability at 600 °C. Moreover, the nickel OMCs offer exceptional activity in the hydrogenation of bulky molecules (∼2 nm).

Ce _0.5 Zr _0.5 O ₂ prepared by the complexing–coprecipitation method (CZ-2) exhibits higher oxygen storage capacity (OSC) and thermal stability than that prepared by coprecipitation (CZ-1) or the complexing–coprecipitation-solution (CZ-3) method. After being aged at 1100 °C for 6 h, CZ-2a exhibited the highest OSC and catalytic activity.