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Vaccination is one of the main advancements in public health in the prophylaxis of infectious diseases. We intend to describe the general knowledge about vaccines/vaccination among Brazilian immigrants in Portugal, characterize their attitudes toward vaccination, and describe their knowledge of the yellow fever (YF) vaccine. A cross-sectional study was conducted using a self-completion questionnaire (face-to-face or remote). A total of 542 people participated in the study; the mean age was 36.81 years; 40.1% were male; 44.8% had their 12th year of schooling; and 27.0% had resided for ≥10 years in Portugal. Regarding general knowledge about vaccination, 53.8% answered at least 6/8 questions correctly. A total of 37.1% tended to have a favorable attitude toward vaccination. Concerning traveling, 76.7% attributed the risk of disease at the destination as the main reason for accepting vaccines. A total of 89.3% knew that there was a risk of YF in Brazil. A total of 40% answered correctly only one question about the YF vaccine; 21.6% did not answer any questions correctly. Thus, most of the Brazilian immigrants in this study have high general knowledge about vaccines/vaccination, few have a favorable attitude, and their knowledge about the YF vaccine is scarce. This could limit vaccination adherence when visiting Brazil, making health education actions necessary to increase knowledge and prevent YF risks.