Electrical sensors have been widely explored for the analysis of chemical/biological species. Ion detection with single charge resolution is the ultimate sensitivity goal of such sensors, which is yet to be experimentally demonstrated. Here, the events of capturing and emitting a single hydrogen ion (H+) at the solid/liquid interface are directly detected using sub–10-nm electrical double layer–gated silicon nanowire field-effect transistors (SiNWFETs). The SiNWFETs are fabricated using a complementary metal-oxide-semiconductor compatible process, with a surface reassembling step to minimize the device noise. An individually activated surface Si dangling bond (DB) acts as the single H+ receptor. Discrete current signals, generated by the single H+-DB interactions via local Coulomb scattering, are directly detected by the SiNWFETs. The single H+-DB interaction kinetics is systematically investigated. Our SiNWFETs demonstrate unprecedented capability for electrical sensing applications, especially for investigating the physics of solid/liquid interfacial interactions at the single charge level.