This data set contains the minimal file necessary to reproduce the DFT calculations contained in the publication: Control of spintronic and electronic properties of bimetallic and vacancy-ordered vanadium carbide MXenes via surface functionalization. the dataset is available on GitLab: https://gitlab.com/praguelab/shuo2019_work1 (Project ID: 13583566) Final Latest tag at moment of submission: https://gitlab.com/praguelab/shuo2019_work1/-/tags/Accepted_manuscript The paper has been received for review on 16th October 2019, and accepted for publication 11th November 2019 in Journal of Physical Chemistry Chemical Physics DOI: 10.1039/c9cp05638f Preprint available on arXiv https://arxiv.org/abs/1910.01509 The work has been financed by Grantova´ Agentura, Univerzita Karlova (Grantova´ Agentura, Univerzita Karlova), OP VVV ‘‘Excellent Research Teams’’, project CUCAM, and International Mobility of Researchers at Charles University (CZ.02.2.69/0.0/0.0/16_027/0008495)