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Simple Summary: Otolith geochemical signatures were important tools used to investigate the population of commercially exploited fish species. Historical and contemporary otolith samples of Isopisthus parvipinnis, Bigtooth corvina, an economically and ecologically important Brazilian fish species, collected in five subareas [São Paulo: North—NSP, Center—CSP and South—SSP; Paraná (PR) and Santa Catarina (SC)] of the shallow waters off the coast of the South Brazil Bight were used in this study. Univariate and multivariate statistical analyses showed spatial differences in otolith chemical composition over the years, suggesting that long-term temporal variability in oceanographic conditions, anthropogenic influence, and climate change on this coastal ecosystem influenced the geochemical signatures. Moreover, these results also confirm that I. parvipinnis is not a single and homogeneous fish stock in this geographic area, supporting the existence of a metapopulation structure scenario and corroborating previous studies that used alternative, complementary phenotypic tags. In this study, otolith geochemical signatures (Element:Ca ratios) were used to investigate the long-term spatial shifts of the population structure of Isopisthus parvipinnis, Bigtooth corvina, an economically and ecologically important Brazilian fish species. Two-hundred and ninety-seven juvenile individuals from historical (1975) and contemporary (2018/2019) samples were collected in five subareas [São Paulo: North—NSP, Center—CSP and South—SSP; Paraná (PR) and Santa Catarina (SC)] of the shallow waters off the coast of the South Brazil Bight were analyzed. The main informative single elements were Co:Ca, Cu:Ca, Li:Ca, Mg:Ca, Mn:Ca, Ni:Ca, Na:Ca, and Rb:Ca. Multivariate analysis showed spatial differences in otolith chemical composition over the years. Samples from 1975 presented an overall low reclassification rate (58%), suggesting the existence of two population units: (1) SP + PR; and (2) SC. However, samples from 2018/2019 discriminated four distinct population units with a good overall reclassification (80%): (1) NSP; (2) CSP; (3) SSP + PR; and (4) SC. This spatial differentiation on the geochemical signatures probably reflects the effects of long-term temporal variability in oceanographic conditions, anthropogenic influence, and climate change on this coastal ecosystem. The data also corroborate and refines the population structure scenario of I. parvipinnis recently described using complementary phenotypic tags. [ABSTRACT FROM AUTHOR]