In this work, we report a favorable diamond substrate to realize semiconductor surface-enhanced Raman spectroscopy (SERS) for trace molecular probes with high sensitivity, stability, reproducibility, recyclability and universality. The boron-doped diamond (BDD) with surface hydrogenation or oxygenation has matched energy levels corresponding to the target molecules and plays a critical role in achieving SERS. The enhancement factor based on BDD substrates can reach 104-105, which approaches those obtained with most nanostructured compound semiconductors and is nearly 3-4 orders of magnitude higher than those of state-of-the-art single-element semiconductors (silicon, germanium, and graphene). The mechanism of SERS is determined to be charge transfer with vibronic coupling, which could enhance the molecular polarizability tensor. Because of its unique properties such as chemical inertness, wide bandgap, modulated doping, surface functionalization, biocompatibility, and high thermal conductivity, the single-element semiconductor diamond can serve a high-performance semiconductor SERS platform with applications in broad fields.