Sugarcane smut, caused by Sporisorium scitamineum, is a globally prevalent disease that severely impacts sugarcane yield and quality. The most cost-effective and sustainable approach to disease control is breeding for smut-resistant varieties. In this study, we conducted a genome-wide association study (GWAS) using a panel of core sugarcane parents and their derived lines to elucidate the genetic basis of smut resistance across seven different environments. We identified 68 new loci significantly associated with smut resistance across all the chromosomes. Based on functional annotations and genomic positions, 164 candidate genes were identified, many of which are related to enzymatic systems, resistance genes, transcription factors, and other pathways implicated in smut defense. Using resistance ratings and associated SNPs, we further selected ten elite parents and derivatives as potential donors for marker-assisted selection (MAS). This study provides a valuable reservoir of genetic resources for improving smut resistance in sugarcane.