This, what har07 posted, should work. In case you need to extend your method a little, I would try to do something like this (though it is not tested, but should work):
(Rebuilt after comment - with Cancellation)
// first define Cancellation Token Source - I've made it global so that CancelButton has acces to it
CancellationTokenSource cts = new CancellationTokenSource();
enum Problem { Ok, Cancelled, Other }; // results of my Task
// cancelling button event
private void CancellButton_Click(object sender, RoutedEventArgs e)
{
   if (this.cts != null)
        this.cts.Cancel();
}
// the main method - I've described it a little below in the text
public async Task<Problem> DownloadFileFromWeb(Uri uriToDownload, string fileName, CancellationToken cToken)
{
   try
   {
       using (Stream mystr = await DownloadFile(uriToDownload))
           using (IsolatedStorageFile ISF = IsolatedStorageFile.GetUserStoreForApplication())
           {
           if (ISF.FileExists(fileName)) return Problem.Other;
           using (IsolatedStorageFileStream file = ISF.CreateFile(fileName))
           {
               const int BUFFER_SIZE = 1024;
               byte[] buf = new byte[BUFFER_SIZE];
               int bytesread = 0;
               while ((bytesread = await mystr.ReadAsync(buf, 0, BUFFER_SIZE)) > 0)
               {
                  cToken.ThrowIfCancellationRequested();
                  file.Write(buf, 0, bytesread);
               }
           }
       }
       return Problem.Ok;
    }
    catch (Exception exc)
    {
       if (exc is OperationCanceledException)
           return Problem.Cancelled;
       else return Problem.Other; 
    }
}
// and download
private async void Downlaod_Click(object sender, RoutedEventArgs e)
{
   cts = new CancellationTokenSource();
   Problem fileDownloaded = await DownloadFileFromWeb(new Uri(@"http://filedress/myfile.txt", UriKind.Absolute), "myfile.txt", cts.Token);
   switch(fileDownloaded)
   {
      case Problem.Ok:
           MessageBox.Show("File downloaded");
           break;
      case Problem.Cancelled:
           MessageBox.Show("Download cancelled");
           break;
      case Problem.Other:
      default:
           MessageBox.Show("Other problem with download");
           break;
    }
}
I've added Cancellation Token - it means that your download operation can be cancelled after Button.Click. On the other hand if await DownloadFile(uriToDownload) is Cancelled it automatically throws OperationCancelled - then you catch that exception and return adequate result.
I haven't run that code, but it may show the main idea.