The present invention discloses a copper-zinc-aluminum-iron single crystal alloy material having an ultra-large grain structure of 5-50 cm grade, obtained by annealing an as-cast alloy having a polycrystalline structure through a single phase region of 800-960° C. for 2-105 h, where the as-cast alloy includes, by weight percentage, 62-82% of copper, 6-29% of zinc, 5-12% of aluminum, and 2-5% of iron. In the present invention, the alloy compositions have an essential difference and are a copper-zinc-aluminum-iron quaternary alloy, and the iron element is an indispensable alloying element. The preparation process of the present invention is extremely simple and very easy to implement and has a very good application prospect.