The present study describes the synthesis of highly active and ordered structures of nickel nanocatalysts by a facile, green, and economically viable approach. The study reveals efficient catalytic activity for the degradation of a number of toxic organic dyes, such as eosin-B (EB), rose bengal (RB), eriochrome black-T (ECBT), and methylene blue (MB). The stable ordered nickel nanostructure (Ni NSs) arrays were prepared via a modified hydrazine reduction route with unique and controlled morphologies in a lyotropic liquid crystalline medium using a nonionic surfactant (Triton X-100). Characterization and optimization studies for the fabricated Ni NSs involving their surface binding interactions, size, and morphologies were carried out using UV-Vis spectroscopy, Fourier transform infrared (FTIR) spectroscopy, X-ray diffraction (XRD), and scanning electron microscopy (SEM).