The mechanical actuation of a (5, 5) single-walled carbon nanotube as a result of added charge is simulated using first-principles calculations. It is observed that while both positive and negative charging tend to expand the nanotube in the axial direction for most levels of charge, radial actuation is less even and symmetric with respect to charge. The spin distribution of the additional charges is investigated, and it is predicted that in some cases unpaired spin configurations are energetically favourable, significantly affecting actuation strains.