This paper investigates customized AA5083 and Al-Mg binary powders produced by gas atomization and assesses cold spray (CS) deposition of these materials with the evaluation of interface quality, deposition efficiency, porosity, and microhardness. While there has been extensive research progress on CS deposition of AA2024, AA6061, and AA7075, less attention has been given to CS 5xxx-series (Al-Mg) aluminum alloys. For the development and investigation of CS Al-Mg series alloys, AA5083 and customized Al-Mg binary powders were fabricated using a close-coupled inert gas atomizer, and those powders were sprayed using a high-pressure cold spray system to produce CS Al-Mg deposits. The microstructural characteristics of the powders, such as lattice constant and the formation of intermetallic networks, were affected by the Mg content of as-atomized powders. Selected CS parameters were able to produce highly dense CS deposits over a range of 1.7-5 wt.% Mg. The Mg content of as-atomized powders also influenced the hardness of the deposits and the DE while having no effect on porosity. The influence of Mg content on powder properties, CS process, and CS Al-Mg deposits has been discussed.