You can analyse mor in details or give a try with an alternate like
(From d in dt1.AsEnumerable
Let c1 = d(0).toString.Trim
Let chk = dt2.AsEnumerable.Any(Function (d2) d2(0).toString.Trim.Equals(c1))
Where not chk
Select r = d).CopyToDataTable
feel free to adapt the 0 to the column name and if needed add more check cols into the match part