We propose and demonstrate nanowire (NW) device platforms on-chip integrated using electric-field-assisted self-assembly. This platform integrates from nanoprobes to microprobes, and conveniently allows for on-chip manipulation, capturing, and electrical characterization of nanoparticles (NPs). Synthesizing segmented (Au–Ag–Au) NWs and aligning them across predefined microelectrode arrays under ac electric field, we controllably form nanogaps between the self-aligned end (Au) segments by selectively removing the middle (Ag) segments. We precisely control and tune the size of this middle section for nanogap formation in the synthesis process. Using electric field across nanogaps between these nanoprobes, we capture NPs to electrically address and probe them at the nanoscale. This approach holds great promise for the construction of single NP devices with electrical nanoprobe contacts.