Let $\hat{n}=(\cos\phi\sin\theta,\sin\phi \sin\theta,\cos\theta)$ i.e. the Cartesian coordinate vector for a point on the unit sphere with polar angle $\theta$ and azimuthal angle $\phi$. By sending a spin-1/2 particle through a Stern-Gerlach device with orientation $\hat{n}$, we can measure the observable
\begin{align}
S_n:=\vec{S}\cdot \hat{n}
&=S_x \cos\phi\sin\theta +S_y \sin\phi \sin\theta+S_z \cos\theta\\ &= \frac{\hbar}{2}\begin{pmatrix} \cos\theta & \cos\phi\sin\theta-i \sin\phi \sin\theta\\ \cos\phi\sin\theta+i \sin\phi \sin\theta & -\cos\theta\end{pmatrix} \\&= \begin{pmatrix} \cos \theta & e^{-i\phi}\sin\theta \\ e^{i\phi}\sin\theta & -\cos\theta\end{pmatrix}
\end{align}
in the $S_z$ basis. The obvious step is now to determine eigenvalues and eigenvectors. But if we denote the spin-up and spin-down eigenstates of $S_z$ as $|0\rangle$ and $|1\rangle$ respectively, then
$$| \psi \rangle = \cos(\theta/2) |0 \rangle + e^{i \phi} \sin(\theta/2)| 1 \rangle=\begin{pmatrix} \cos(\theta/2)\\ e^{i\phi}\sin(\theta/2)\end{pmatrix}$$ and therefore
\begin{align}
S_n |\psi\rangle
&= \frac{\hbar}{2}\begin{pmatrix} \cos \theta & e^{-i\phi}\sin\theta \\ e^{i\phi}\sin\theta & -\cos\theta\end{pmatrix}\begin{pmatrix} \cos(\theta/2)\\ e^{i\phi}\sin(\theta/2)\end{pmatrix} \\
&= \frac{\hbar}{2}\begin{pmatrix} \cos(\theta)\cos(\theta/2)+\sin(\theta)\sin(\theta/2)\\ e^{i\phi}[\sin(\theta)\cos(\theta/2)-\cos(\theta)\sin(\theta/2)]\end{pmatrix}\\
&= \frac{\hbar}{2}\begin{pmatrix} \cos(\theta/2)\\ e^{i\phi}\sin(\theta/2)\end{pmatrix}=+\frac{\hbar}{2}|\psi\rangle
\end{align}
where in the second-to-last equality I've used the trigonometric product-to-sum formula. Hence $|\psi\rangle$ is the $S_n=+\hbar/2$ eigenstate. In other words: If a spin-1/2 particle passes through an SG device with orientation $\hat{n}$ and comes out deflected up, then $|\psi\rangle$ is the resulting spin state. (Correspondingly, one can show that $S_{-n}|\psi\rangle=-\hbar/2|\psi\rangle$ i.e. $|\psi\rangle$ will deflect down if the SG device is flipped.) The upshot is that $\theta,\phi$ are not angles in Hilbert space; rather, they're the angles in real space for the SG device for which $|\psi\rangle$ is the spin state of the upward-deflected beam.
Note that the above description is limited to points on the surface of the Bloch sphere i.e pure states. For points on the interior of the Bloch sphere, we need to go to the density matrix formalism as presented by gLs and I'll defer to that answer.