Low-dimensional materials have aroused widespread interest for their novel and fascinating properties. Based on first-principles calculations, we predict the one-dimensional (1D) InSeI nanochains with van der Waals (vdW) interchain interactions, which could be exfoliated mechanically and kept at steady states at room temperature. Compared with bulk InSeI, the single nanochain InSeI has a larger direct bandgap of 3.15 eV. Its calculated carrier mobility is as high as 54.17 and 27.49 cm2 V-1 s-1 for holes and electrons, respectively, comparable with those of other 1D materials. In addition, a direct-to-indirect bandgap transition is implemented under a small applied strain (∼6%). More importantly, the nanochains are found to be promising candidates for optoelectronic devices since they possess a high absorption coefficient of ∼105 cm-1 in the ultraviolet region. The results thus pave a novel avenue for the applications of InSeI nanochains with excellent thermal stability in nanoelectronic and optoelectronic devices.