If you mean the observable functioning of our brain, i.e. our
behaviour, then no, being computational doesn't necessarily imply predictability; there is a complexity problem - we can't know the initial state and connectivity, nor map all the inputs precisely enough to predict what it will do. There is also the chaos problem - parts of the brain apparently function chaotically, and it is often said (I'm not sure how accurately) that the whole brain operates on the edge of chaos; if there is any chaotic function involved, there will be inherent unpredictability.
Having said that, for obvious reasons our gross behaviour is fairly predictable most of the time.
I think QM has quashed the idea of a fundamentally deterministic reality, but if we assume that this is statistically averaged out to deterministic equivalence at the macro levels of cells and above, then I think one could take a deterministic viewpoint. If not, then we need to make some allowance for stochastic 'interference'.
But whether reality is deterministic or stochastic, uncertainty, creativity, and free will are abstractions, human constructs. They exist as interpretations we make of what we perceive of reality. Asking if such an abstraction is an illusion opens a semantic can of worms. Before we can answer that, we need to agree on a clear definition of what we mean by it. Good luck with 'free will'
Neurons are complex and dynamic biological systems, so their responses are not entirely consistent, but if you know the initial state and environment well enough you can predict pretty well how and when it will respond to various stimuli, both in-vitro and in-vivo. A lot of work has been and is being done on this. Google is your friend here.