The discharge of toxic dye effluents from industry is a major concern for environmental pollution and toxicity. These toxic dyes can be efficiently removed from waste streams using a photocatalysis process involving visible light. Due to its simple synthesis procedure, inexpensive precursor, and robust stability, graphitic carbon nitride (g-C3N4, or CN) has been used as a visible light responsive catalyst for the degradation of dyes with mediocre performance because it is limited by its low visible light harvesting capability due to its wide bandgap and fast carrier recombination rate. To overcome these limitations and enhance the performance of g-C3N4, it was coupled with a narrow bandgap copper tin sulfide (CTS) semiconductor to form a p-n heterojunction. CTS and g-C3N4 were selected due to their good stability, low toxicity, ease of synthesis, layered sheet/plate-like morphology, and relatively abundant precursors. Accordingly, a series of copper tin sulfide/graphitic carbon nitride nanocomposites (CTS/g-C3N4) with varying CTS contents were successfully synthesized via a simple two-step process involving thermal pyrolysis and coprecipitation for visible-light-induced photocatalytic degradation of methyl orange (MO) dye. The photocatalytic activity results showed that the 50%(wt/wt) CTS/g-C3N4 composite displayed a remarkable degradation efficiency of 95.6% for MO dye under visible light illumination for 120 min, which is higher than that of either pristine CTS or g-C3N4. The improved performance is attributed to the extended light absorption range (due to the optimized bandgap), effective suppression of photoinduced electron-hole recombination, and improved charge transfer that arose from the formation of a p-n heterojunction, as evidenced by electrochemical impedance spectroscopy (EIS), photocurrent, and photoluminescence results. Moreover, the results of the reusability study showed that the composite has excellent stability, indicating its potential for the degradation of MO and other toxic organic dyes from waste streams.