Graphitic carbon nitride (g-C3N4) has been widely used in various photocatalyst applications. However, compared with conventional metal-based photocatalysts, it exhibits low photocatalytic activity because of the low mobility of its charge carriers. In this study, g-C3N4/nanodiamond (ND) nanocomposites were fabricated via a facile single-step heating strategy. Under visible-light irradiation, the optimal g-C3N4/ND nanocomposites with 1.0 wt% ND content exhibited an RhB degradation rate more than two times greater than that of the g-C3N4. In addition, reutilization experiments showed that the g-C3N4/ND nanocomposites exhibit good stability and reusability. This remarkable enhancement of the photocatalytic activity was attributed to the interfacial effect between g-C3N4 and ND, which reduces energy-wasteful electron–hole recombination and promotes charge-separation efficiency. Such an approach could accelerate the development of composites for photocatalyst applications and provide more rational guidance and fundamental understanding toward realizing the theoretical limits of interfaces.