Photocatalysis involves the excitation of semiconductor materials by light absorption to produce electron-hole pairs, following charge-pair separation to induce the oxidation of organic pollutants. [1b] Among various semiconductors, oxides of the elements Ti, Bi, Zn, and Sn are preferable materials for photocatalytic processes. [1a] However, most of them generally show poor efficiency in photocatalytic reactivity due to wide band gaps of the materials and relatively high recombination rates of electron-hole pairs. Various promising approaches using composite materials, morphology control, noble metal loading, and heterostructural construction have been explored to enhance photocatalytic activity of the semiconductor materials. [1a] However, these strategies often require complicated preparation procedures. Therefore, the search for simple compounds with an enhanced ability to degrade organic pollutants has been the focus in photocatalytic research area. Recently, graphitic carbon nitride (g-C 3 N 4 ) with a stacked 2D structure has received much attention as a metal-free semiconductor and is rapidly becoming a favorite in material science. With medium band gap and thermal/chemical stability in an ambient environment, g-C 3 N 4 has become one of the most promising photocatalytic materials. [2] More importantly, doping with metal ions or nonmetal ions to form active sites for optimal heterojunctions leading to modify the band gap and morphology has been achieved for efficient separation of pairs electrons and holes to enhance the photocatalytic performance of g-C 3 N 4 significantly. A number of studies on the photocatalytic performance of g-C 3 N 4 have been reported to date. [3] Layered double hydroxides (LDHs), a group of layered functional materials with a special octahedral microstructure, have the following major features: the chemical composition of the layers is adjustable, the type and number of interlayer anions is exchangeable, and the particle size distribution is controllable. [4] Recently, LDHs have received worldwide attention because of their multiple applications, such as adsorbents, [5] catalysts, and catalytic supports. [6] The general formula of LDHs is [M 1−x 2+ M x 3+ (OH) 2 ] x+ (A n− ) x/n : yH 2 O, where M 2+ and M 3+ are divalent (Ca 2+ , Mg 2+ , Zn 2+ , Ni 2+ , Cu 2+ ) and trivalent (Al 3+ , Fe 3+ , Cr 3+ ) metal Novel photocatalysts in the form of zinc oxide-zinc bismuth oxide (mixedmetal oxide [MMO]) and graphitic carbon nitride (CN) hybrid composites are developed via a co-precipitation method followed by calcination at 520 °C. The as-prepared MMO-CN hybrid composites are evaluated on the basis of their photocatalytic activities for Rhodamine B (RhB) in aqueous solutions under visible light irradiation. The strong electronic coupling between two components within the MMO-CN heterostructure, which suppresses the photogenerated recombination of electrons and holes to a remarkable extent, is revealed. The prepared composites exhibit an excellent photocatalytic activity, leading to mo...