We next explored the coupling reaction between amide 5 and various aromatic carbonyl compounds 7, including aldehyde, ketone, and ester (Figure ). Attaching photogenerated radical intermediates to C=O bonds is challenging and was achieved only in limited instances, for example, via the reaction between an organochromium-type carbanion species and aldehydes. Using CdS QD gels as the photocatalyst, we successfully coupled N,N-dimethylacetamide (DMA) with benzaldehyde (8a), acetophenone (8b), 4fluorobenzophenone (8c), and dimethyl terephthalate (8d) in moderate to excellent yields of 28% to 78%. The reaction between N,N-dimethylacetamide and dimethyl terephthalate also led to 6% of ketone product (Figure ). Most impressively, we observed an unusual three-component reaction between N,N-dimethylacetamide, acetone, and dimethylterephthalate, forming an alkylated pinacol C-C cou-pling product 9 at a good yield of 42%. The above results have clearly demonstrated that CdS QD gels are a versatile photocatalyst for activating C-H bonds and efficiently utilizing the generated intermediates for coupling reactions.