I may be misreading the original post, but it seems like he has a dvd ripped to the hard drive that is larger than what can be directly burned to a single layer dvd. If this is the case, there are several things you can do.
First, you could take out extras and additional soundtracks, and just copy the main movie. You can do this with DVDShrink in reauthor mode. You might still have to use a little compression on the main movie. There are plenty of guides to DVDShrink available, so look through a couple. You can find some at mrbass.org, videohelp.com and here at cdfreaks too. DVDShrink is a free program and can be downloaded from mrbass.org
If you want the entire movie and don't object to a little more compression, you can use DVDShrink for the whole thing. Shrink can output to regular dvd files that you can burn with Nero or you can output to an ISO and use ImgBurn, which is my favorite burning application for video. ImgBurn is a free tool.
The last option is to burn the entire dvd, uncompressed, to a dual layer dvd. (assuming it is too large to fit onto a single layer) My normal method to do this is to rip from the original dvd to the hard drive using DVDDecrypter in ISO Read Mode. This will give you an ISO file and a very small MD5 file. Load the md5 file into ImgBurn in Write mode and it will burn to a dual layer disk and keep the layer break set correctly.
If you want to start with the files you have now---and burn to a dual layer disk, then you could use ImgBurn in Build mode. It will make an ISO file for you and automatically try to set the layer break correctly when you burn to the disk. In Build mode, you can have ImgBurn output to an ISO on the hard drive, or just go directly to your burner. Read some information on the use of the program at the forums for ImgBurn.
And there is one more bit to remember. If you are burning to a dual layer disk, only use Verbatim +R disks. They are the only reliable dual layer disks that are commonly available.