The contamination of water with organic pollutants, such as dyes, has become a serious threat to the environment. Therefore, the development of a cost-effective, eco-friendly, proficient, and visible-light-driven catalyst for the treatment of organic dye-contaminated wastewater has been a burning issue recently. Photocatalysis is suggested as a potential treatment technique for the eradication of organic pollutants. The 1D tunnel-structured manganese oxide octahedral molecular sieve (OMS) is a suitable substance to be tested as a visible-light-driven photocatalyst for the degradation of organic contaminants. However, the fast recombination of photoinduced charges (h+/e−) limits its photocatalytic application. The development of heterojunctions between OMS and other metals, such as Ag, is a suitable technique for improving the photocatalytic performance of OMS. In this study, Ag-OMS with plasmon-enhanced photocatalytic activity is reported for the photodegradation of crystal violet dye. Manganese oxide OMS was prepared by an acidic precipitation method using potassium permanganate, manganese acetate, and nitric acid as precursor materials. Ag nanoparticles were deposited on OMS using leaf extracts of Calotropis gigantea. The deposition of Ag enhanced the photocatalytic performance of OMS from 68 to 95%. The effects of Ag contents, catalyst dosage, and concentration of crystal violet dye on catalytic performance were explored as well. Approximately 100, 95, and 75% photodegradation of 50, 100, and 150 mg/L crystal violet dye was observed in 90, 120, and 120 min in the presence of 10% Ag-OMS, respectively. Excellent photocatalytic performance, low dose utilization, and reusability proved that Ag-OMS might have practical environmental applications.