Because they have some quite serious doctrinal differences with the official Masoretic Text, and that causes some discomfort. The fact that most of the LXX differences are supported by both the Samaritan Pentateuch and the Dead Sea Scrolls, of course, causes even more discomfort.
The problem is that the oldest masoretic text is far newer than either the Greek or the Latin manuscripts that we possess.
And far newer than the LXX.
We know for a fact that Jerome had access to Hebrew manuscripts that are not at present extant. Which needs to be taken into consideration.