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Scope: Some very-low density lipoprotein (VLDL) properties may render them more pro-atherogenic. We aimed to assess whether a Mediterranean diet (MedDiet) or an energy-reduced MedDiet with increased physical activity improves them. Methods and results: In a sample of the PREvención con DIeta MEDiterránea (PREDIMED) study, a 1-year intervention with MedDiet with extra-virgin olive oil (n = 89) or nuts (MedDiet-Nuts; n = 79) is compared with a low-fat diet (n = 90). In the PREDIMED-Plus study, a 1-year intervention with energy-reduced MedDiet and physical activity (n = 103) is compared with an ad libitum MedDiet (n = 101). VLDL levels of apolipoprotein C-I, C-III, triglycerides, and cholesterol; the apolipoprotein E-/C-I ratio; and VLDL ex-vivo triglyceride transfer are measured. In PREDIMED participants in both MedDiet groups combined, VLDL apolipoprotein C-III levels are nominally reduced (-0.023 SD units, 95% CI -0.44 to -0.014, p = 0.037). VLDL triglyceride transfer is nominally increased in the MedDiet-Nuts group (+0.39 SD units, 95% CI 0.012-0.78, p = 0.045). In PREDIMED-Plus, no inter-group differences are detected. Conclusions: In older adults at high cardiovascular risk, MedDiet is associated with lower VLDL atherogenicity versus a low-fat diet. No differences are seen after an energy-reduced MedDiet with physical activity. The authors want to thank Daniel Muñoz-Aguayo, Gemma Blanchart, and Sònia Gaixas for their laboratory support, and Stephanie Lonsdale for her help in editing the English text. A full list of names of all PREDIMED and PREDIMED-Plus study collaborators is available in the Supporting files Appendix 1. The authors also thank the PREDIMED-Plus Biobank Network as a part of the National Biobank Platform of the ISCIII for storing and managing the PREDIMED-Plus biological samples. CIBER de Fisiopatología de la Obesidad y Nutrición (CIBEROBN) is an initiative of Instituto de Salud Carlos III (Madrid, Spain), and is financed by the European Regional Development Fund. Acknowledgements to European Research Council (Grant 340918). This work was supported by the Instituto de Salud Carlos III (grant numbers: IFI20/00002, PI19/00017, PI15/00047, PI18/00020, PI16/00533, PI13/00233, PI21/00024, PI20/00012, and CP21/00097) and co-funded by the European Union. The funders played no role in study design, collection, analysis, or interpretation of data, and neither in the process of writing the manuscript and the publish process.