1. It's tricky to scale out a Redis node when it gets too big. Because RDB files are just a single dump of all data, it's not easy to make a specific partitioning of the dataset. This was a very important requirement for us in order to ease scaling (redis-cluster wasn't ready yet -- we've been following that carefully).
2. When you store hundreds of GB of persistent data in Redis, the startup process can be very slow (restoring from RDB/AOF). Since it can't serve reads or writes during this time, you're unavailable (setting up a slave worsens the following problem).
3. The per-key overhead in Redis (http://stackoverflow.com/questions/10004565/redis-10x-more-m...). We have many billions of sets that are often only a few elements in size -- think of slicing data by city or device type -- which means that the resulting overhead can be larger than the dataset itself.
If you think about these problems upfront, they're not too difficult to solve for a specific use case (partition data on disk, allow reads from disk on startup), but Redis has to be generic and so can't leverage the optimizations we made.