I'm not sure what kind of "bond" you're looking for, but I think you'll be disappointed.
Axolotls have a brain the size of a pea. They won't love you - they can't.
They can get used to you. For that, hand feeding is indeed a good method. They'll come to associate big moving things with food, and will eventually react excited if you stick your hand in the water. Similarly, big shapes moving around outside the glass will make them think "food!".
Once they're used to you they might not even mind being touched (though you shouldn't touch them often - it's not good for their skin)
If you want, you can even confuse that with affection.
They're not really pets to play or cuddle with, however.
You can certainly keep them busy with food (hiding it, moving it), which I think is very healthy for any pet. You won't "bond" more than the bond between a predator and easy prey (with you being the easy prey).