I am trying to learn some spin geometry stuff and getting a bit confused. The unit quaternions can be thought of as a group structure on $S^3$ which gives the group $\text{Spin}(3)$.
Is there some sense in which $S^3$ is isomorphic to or equal to $\text{Spin}(3)$?
Yes. This group appears to possess a bunch of alternative definitions, like
See https://en.wikipedia.org/wiki/Spin_group#Accidental_isomorphisms