What makes quantities in physics important is that they are useful. What makes them useful is the equations that they obey. In classical physics, the angular momentum (defined in terms of components as $L_{i}=\epsilon_{ijk}x_{j}p_{k}$) turns out to be useful in a lot of situations. It transforms like a (pseduo-)vector, and—even more importantly—in some fairly natural systems it is conserved. A particularly well known example is that, for a particle moving in a central potential $V(\vec{x})$, $\vec{L}$ is conserved, according to the classical equations of motion. (The conservation of $\vec{L}$ may be demonstrated in many ways, such as via the fact that $\{L_{i},H\}=0$, where $\{\cdot,\cdot\}$ is the Poisson bracket and $H$ is the Hamiltonian.)
With the transition to quantum mechanics, it will initially be an open question whether the operator with components $\hat{L}_{i}=\epsilon_{ijk}\hat{x}_{j}\hat{p}_{k}$ will still be the "right" expression for the angular momentum. That $\hat{L}_{i}$, so defined, must at least be part of the angular momentum in the quantum theory, because the classical and quantum expressions must correspond in the classical limit (taking $\hbar\rightarrow0$). However, there is no a priori reason why there cannot be additional intrinsically quantum mechanical contributions to the angular momentum,
$$\hat{L}_{i}=\epsilon_{ijk}\hat{x}_{j}\hat{p}_{k}+\hat{M}_{i},$$
where the operator $\hat{M}$ is at least $\mathcal{O}(\hbar)$. What ultimately decides which expression for the angular momentum is the "right" one is which expression is most useful. It turns out that in nonrelativistic quantum mechanics, the naively chosen $\hat{L}_{i}=\epsilon_{ijk}\hat{x}_{j}\hat{p}_{k}$ is still a conserved quantity, since it commutes with the Hamiltonian, $[L_{i},H]=0$; this is directly analogous to the classical theory. The fact that $\hat{L}^{2}$ and $\hat{L}_{z}$ commute with $H$ is something that we take advantage of when solving the problem of a particle in central potential. Those two operators can be diagonalized simultaneously with $H$, and their eigenvalue are consequently "good" quantum numbers that can be used as part of the parameterization of the eigenvalue and eigenstate spectrum. So this definition of the angular momentum operator turns out to be very useful, and that is why we use it in nonrelativistic quantum mechanics.
However (although it is not usually discussed in these terms), the situation changes in relativistic quantum mechanics. For the Dirac equation with a central potential, it turns out that $\hat{L}_{i}=\epsilon_{ijk}\hat{x}_{j}\hat{p}_{k}$ does not commute with the full Hamiltonian. Instead, it behooves us to define a different quantity to be the angular momentum,
$$\hat{J}_{i}=\epsilon_{ijk}\hat{x}_{j}\hat{p}_{k}+\frac{\hbar}{2}\hat{\Sigma}_{i}.$$
This, of course, has exactly the form hypothesized above, with the intrinsically quantum contribution $\hat{M}_{i}$ now being nonzero. The operator $\hat{M}_{i}=\frac{\hbar}{2}\hat{\Sigma}_{i}$ is not constructed out of the position and momentum variables; instead it is a matrix operator, acting in the space of Dirac spinors. By convention, we still call the first term, $\epsilon_{ijk}\hat{x}_{j}\hat{p}_{k}$ the "orbital angular momentum" component $\hat{L}_{i}$; the new term is the "spin angular momentum." However, it is the total angular momentum $\hat{J}_{i}$ which is conserved and so ultimately the most important (labeling the energy eigenstates, for example).