I'd say you've answered your own question here.
I have a good reason to use mongodb
for part of my app.
Assuming you also have a good reason for keeping other parts in MySQL, I would say the answer is yes. Your question implies (at least to me) that you have a good and well-researched understanding of the various options and their strengths and weaknesses and have therefore reached a sensible conclusion in that splitting your models is doable.
Assuming the two halves are not linked in some way (relationships between the two sounds like a recipe for pain later), I would suggest that you go for it and use each tool for what it is best at.
It is possible to address some of the concerns Michael raises with this approach. since you are focusing on using Rails, you can use ActiveRecord for your MySQL-based models and use MongoMapper for your MongoDb based models. This way, you won't have to deal with two completely different querying methods since MongoMapper provides a very ActiveRecordish approach. Of course, you can easily drop down into Mongo-specific querying as and when you need to.
The concern regarding relationships cross-DB are valid in my opinion and if this is something you'd end up having a lot of, I would definitely advise examining the situation to make sure this is something you're happy to live with. I imagine you might be saving up a lot of pain for later in that particular case.
Overall, I'd suggest that as long as your two halves are relatively disconnected from each other, a split-personality persistence layer will work well for you.