Voldemort's support for adding nodes was just added recently (this month). So I would expect Cassandra's to be more robust given the longer time to cook and a larger community testing.
Both are fast (> 10k ops/s per machine). Because of their storage designs, I would expect Cassandra to be faster at writes, and Voldemort to be faster at reads. I would also expect Cassandra's performance to degrade less as the amount of data per node increases. And of course if you need more than just a key/value data model Cassandra's ColumnFamily model wins.
I don't know of any head-to-head benchmarks since the one done for NoSQL SF last June, which found Cassandra to be somewhat faster at whatever workload mix he was using. (The "vpork" talk from http://blog.oskarsson.nu/2009/06/nosql-debrief.html) 8 months is an eternity with projects under this much development, though.