Ab ifunctional 3d-metal catalyst for the cascade synthesis of diverse pyrroles from nitroarenes is presented. The optimal catalytic system Co/NGr-C@SiO 2-L is obtained by pyrolysis of ac obalt-impregnated composite followed by subsequent selective leaching.I nt he presence of this material, (transfer) hydrogenation of easily available nitroarenes and subsequent Paal-Knorr/Clauson-Kass condensation provides > 40 pyrroles in good to high yields using dihydrogen, formic acid, or aC O/H 2 Om ixture (WGSR conditions) as reductant. In addition to the favorable step economy,this straightforward domino process does not require any solvents or external cocatalysts.The general synthetic utility of this methodology was demonstrated on avariety of functionalizedsubstrates including the preparation of biologically active and pharmaceutically relevant compounds,for example,(+ +)-Isamoltane.