Whilst I think that the DSS are certainly the largest
collection of the Tanakh found in antiquity, IIRC, there are a few older Hebrew, and Greek, fragments going quite far back.
Oddly, Wikipedia has a good article on this: http://tinyurl.com/65qhwx2
Apparently the oldest known fragment of the Tanakh is a 600BCE Good-luck charm inscribed with the priestly blessing from Numbers 6:24–27.
The oldest fragments from the Greek Septuagint date to the 2nd Century BCE