Creatine (Cr) is an essential metabolite in the creatine kinase reaction, which plays a critical role in maintaining normal cardiac function. Chemical exchange saturation transfer (CEST) MRI offers a novel way to map myocardium Cr. This study aims to investigate the dynamic alteration in myocardium Cr during acute infarction using CEST MRI, which may facilitate understanding of the heart remodeling mechanism at the molecular level. Seven adult Bama pigs underwent cardiac cine, Cr CEST, and late gadolinium‐enhanced (LGE) T1‐weighted (T1w) imaging three and 14 days after myocardial infarction induction on a 3 T scanner. Cardiac structural and functional indices, including myocardium mass (MM), end‐diastolic volume (EDV), end‐systolic volume (ESV), stroke volume (SV), and ejection fraction (EF), were measured from cines. Infarct angle was determined from LGE T1w images, based on which myocardium was classified into infarct, adjacent, and remote regions. Cr‐weighted CEST signal was quantified from a three‐pool Lorentzian fitting model and measured within each region and the entire myocardium. Student's t‐test was conducted to evaluate any significant differences in measurements between the two time points. Correlation was assessed with Pearson correlation. P values less than 0.05 were considered statistically significant. Over the studied period, MM, EDV, and ESV did not alter significantly (P > 0.05), whereas significant increases of SV and EF and decrease of infarct angle were observed (P < 0.05). Meanwhile, the Cr‐weighted CEST signal elevated significantly on Day 14 compared with Day 3 in the infarct (10.00 ± 1.28% versus 6.91 ± 1.54%, P < 0.01), adjacent (11.17 ± 2.00% versus 8.01 ± 1.58%, P = 0.01), and entire myocardium (11.03 ± 1.36% versus 8.19 ± 1.28%, P < 0.01). Moderate negative correlations were shown between the infarct angle and Cr‐weighted CEST signals in the infarct (r = −0.80, P < 0.001), adjacent (r = −0.58, P = 0.03), and entire myocardium (r = −0.76, P < 0.01). In conclusion, the dynamic increase of myocardium Cr during acute infarction may interact with cardiac structural and functional recovery. The study provides supplementary insights into the heart remodeling process from the metabolic viewpoint. Significant increase of myocardium creatine was shown during acute infarction using chemical exchange saturation transfer MRI, exhibiting association with cardiac structural and functional recovery. The study provides supplementary insights into the heart remodeling process at the molecular level.