Ceramic-metallics (cermets) have emerged as an important class of composite material combining favorable properties of their constitutive phases. In this work, nanostructured cermet Ni(Zn)–Al2O3 composition was synthesized using the high-energy mechanical alloying (HE-MA) method to be deployed as a cold spray deposition powder feedstock. Pre-milled Ni(Zn) alloy particles were mechanically mixed followed by milling in a SPEX™ 8000 M High Energy Ball Mill at a fixed 1050 rpm. The material design-of-experiment (DoE) involved two design compositions (30 wt% and 50 wt% α-alumina) with two substitutional alloy compositions, Ni(5 wt%Zn) and Ni(10 wt%Zn), along with milling time as a process variable. Microstructural characterization confirmed the embedment of nanoscale Al2O3 grain in micron-scale Ni(Zn) alloy particles. Additionally, EBSD analysis of Ni(Zn) alloy particles revealed that Ni(5 wt%Zn) experienced more uniform plastic deformation, work hardening and subsequent fracturing when compared to Ni(10 wt% Zn) alloy particles. The particle size measurement was carried out by laser diffraction showed that the cermet particles milled for 4 h had the desired size range for the objective of cold spraying. Also, the embedment of alumina into the Ni(Zn) alloy matrix and thereby, homogenization of cermet particles enhanced with the increase in milling time.