What I propose here could possibly be simplified further, but that's at least a first direction.
First, any unitary can be written as $U=e^{-it/\hbar \widetilde{H}}$ for some $t$ and $\widetilde{H}$ (the Hamiltonian) hermitian which we can rewrite $U=e^{-i H}$ where $H$ is also Hermitian.
Then, the $n$-Pauli matrices form a basis for any operator acting on $n$ qubits.
For this reason, $H=\sum_{i_1...i_n} \alpha_{i_1...i_n} \sigma_{i_1} \otimes ... \otimes \sigma_{i_n}$ with $\alpha_{i_1...i_n}$ a real coefficient, and $\sigma_k$ being equal to the identity matrix in two dimensions for $k=0$, or $X$ for $k=1$, $Y$ for $k=2$, $Z$ for $k=3$.
In general, an $n$-qubit unitary matrix can then be written as:
$$U=e^{-i \sum_{i_1...i_n} \alpha_{i_1...i_n} \sigma_{i_1} \otimes ... \otimes \sigma_{i_n}}$$
Your question is a particular case for $n=2$.
Now it might not be exactly the question you ask as you would probably like to have it in an non exponentiated form. Also, I guess that some symmetries could be exploited to simplify my answer (for instance a global phase doesn't matter).
But maybe that's still somewhat usefull for you, I don't know.