Metal halide perovskite (MHP) nanocrystals (NCs) have emerged as promising materials for various optoelectronic applications including photovoltaics, light-emitting devices, and photodetectors because of their high absorption coefficient, high diffusion length, and photoluminescence quantum yield. However, understanding the morphological evolution of the MHP NCs as well as their controlled assembly into optoelectronic devices is still challenging and will require further investigation of the colloidal chemistry. In this study, we found that the amount of n-octylamine (the capping agent) plays a crucial role in inducing further growth of the MHP NCs into one-dimensional nanowires during the aging process. In addition, we demonstrate that the dielectrophoresis process can permit self-alignment of the MHP nanowires with uniform distribution and orientation on interdigitated electrodes. A strong light-matter interaction in the MHP NWs array was observed under UV illumination, indicating the photo-induced activation of their luminescence and electrical current in the self-aligned MHP nanowire arrays.