first make a DataTable from current ComboBox DataSource:
DataTable dt =(DataTable) comboBox1.DataSource;
then find target item in DT and remove it from DT.
then set again DT for comboBox datasourse:
DataTable dt = (DataTable)comboBox1.DataSource;
DataRow dr = dt.Rows.Find("TargetKey");
dt.Rows.Remove(dr);
comboBox1.DataSource = dt;