The only way I know would be to call TableControl.Model.ColWidths.ResizeToFit on each of the tables. Here is a button handler that does this for a 3 tables releated tables, parent, child and grandchild.
private void button1_Click(object sender, System.EventArgs e)
{
this.gridGroupingControl1.BeginUpdate();
GridTableDescriptor parentTD = this.gridGroupingControl1.TableDescriptor;
GridTableControl tc = this.gridGroupingControl1.GetTableControl(parentTD.Name);
tc.Model.ColWidths.ResizeToFit(GridRangeInfo.Table());
GridTableDescriptor childTD = parentTD.Relations["ParentToChild"].ChildTableDescriptor;
tc = this.gridGroupingControl1.GetTableControl(childTD.Name);
tc.Model.ColWidths.ResizeToFit(GridRangeInfo.Table());
GridTableDescriptor gridChildTD = childTD.Relations["ChildToGrandChild"].ChildTableDescriptor;
tc = this.gridGroupingControl1.GetTableControl(gridChildTD.Name);
tc.Model.ColWidths.ResizeToFit(GridRangeInfo.Table());
this.gridGroupingControl1.EndUpdate(true);
}