I eventually stumbled upon an example of the usage I was looking for – to assign an error to the Model in general, rather than one of it’s properties, as usual you call:
ModelState.AddModelError(string key, string errorMessage);
but use an empty string for the key:
ModelState.AddModelError(string.Empty, "There is something wrong with Foo.");
The error message will present itself in the <%: Html.ValidationSummary() %>
as you’d expect.