You need a loop for your rows :
System.Data.DataTable dttxfile = new System.Data.DataTable();
da2.Fill(dttxfile);
DataColumnCollection dcCollection = dttxfile.Columns;
Microsoft.Office.Interop.Excel.ApplicationClass ExcelApp = new Microsoft.Office.Interop.Excel.ApplicationClass();
ExcelApp.Application.Workbooks.Add(Type.Missing);
for(int ii=1 ; ii< dttxfile.Rows.Count+1; ii++)
for (int j = 1; j < dttxfile.Columns.Count + 1; j++)
{
if(ii==1)
ExcelApp.Cells[ii, j] = dcCollection[j-1].ToString();
ExcelApp.Cells[ii + 1, j] = dttxfile.Rows[ii - 1][j - 1].ToString();
}