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Metabolic modulation is a promising therapeutic approach to prevent adverse remodeling after MI. However, whether material\u2010derived cues can treat MI through metabolic regulation is mainly unexplored. Herein, a Cu<jats:sup>2+<\/jats:sup> loaded casein microgel (CuCMG) aiming to rescue the pathological intramyocardial metabolism for MI amelioration is developed. Cu<jats:sup>2+<\/jats:sup> is an important ion factor involved in metabolic pathways, and intracardiac copper drain is observed after MI. It is thus speculated that intramyocardial supplementation of Cu<jats:sup>2+<\/jats:sup> can rescue myocardial metabolism. Casein, a milk\u2010derived protein, is screened out as Cu<jats:sup>2+<\/jats:sup> carrier through molecular\u2010docking based on Cu<jats:sup>2+<\/jats:sup> loading capacity and accessibility. CuCMGs notably attenuate MI\u2010induced cardiac dysfunction and maladaptive remodeling, accompanied by increased angiogenesis. The results from unbiased transcriptome profiling and oxidative phosphorylation analyses support the hypothesis that CuCMG prominently rescued the metabolic homeostasis of myocardium after MI. 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