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DataGridViewComboBoxColumn bb = new DataGridViewComboBoxColumn();
bb.DataSource = dt;
bb.HeaderText = "名称";
bb.DisplayMember = "NAME";
bb.ValueMember = "ID";
bb.DataPropertyName = "ID";
grd1.Columns.Add(bb);
DataGridViewCell cell = this.dataGridView1.Rows[0].Cells[0];
cell.Value = 2;
看来你只能遍历一下行,给它赋值了