To preface, I have little background in representation and Lie theory.
My understanding is as such: Given any finite dimensional Hilbert space $\mathcal{H}$ and representation $\rho: SU(2) \rightarrow GL(\mathcal{H})$, due to the compactness of $SU(2)$ the representation $\rho$ is completely reducible. That is $\rho \cong \bigoplus_i \rho_i$ where each $\rho_i$ is an irreducible representation of $SU(2)$ over some invariant subspace $\mathcal{H}_i$. These irreducible representations are characterized by the dimension of their (invariant) representation space and so are unique up to isomorphism. We identify each irreducible representation with a spin value.
My question is: what is the physical evidence that tells us $SU(2)$ is the right group to use to model non-relativistic spin?