A novel composite consisting of NiO/NiC/g-C₃N₄ with excellent photocatalytic properties was successfully synthesized by the simple calcination of layered double metal hydroxide (LDH) and melamine. The color and chemical composition of the as-prepared composites could be tailored by changing the mass ratio of NiAl-LDH and g-C₃N₄. For the L4C composite at the ratio of 1 : 1, it showed the desired dark color due to the generated NiC. It also showed high photodegradation efficiency under visible light irradiation, reaching 97.5% toward Rhodamine B and 92.6% toward tetracycline. The high photodegradation efficiency could be mainly attributed to the unique formation of NiC cocatalysts coupled with g-C₃N₄ and NiO semiconductors, which constructed a Z-scheme system and facilitated the efficient separation of the photogenerated electron–hole pairs. The present findings provide a promising approach for fabricating the new types of composite photocatalysts for pollutant degradation.