The lithium amide (LiNH2) + lithium hydride (LiH) system is one of the most attractive light-weight materials options for hydrogen storage. Its dehydrogenation involves mass transport in the bulk (amide) crystal through lattice defects. We present a first-principles study of native point defects and dopants in LiNH2 using density functional theory. We find that both Li-related defects (the positive interstitial Li+i and the negative vacancy V−Li) and H-related defects (H+i and V−H) are charged. Li-related defects are most abundant. Having diffusion barriers of 0.3–0.5 eV, they diffuse rapidly at moderate temperatures. V−H corresponds to the [NH]2− ion. It is the dominant species available for proton transport with a diffusion barrier of ∼0.7 eV. The equilibrium concentration of H+i, which corresponds to the NH3 molecule, is negligible in bulk LiNH2. Dopants such as Ti and Sc do not affect the concentration of intrinsic defects, whereas Mg and Ca can alter it by a moderate amount. Ti and Mg are easily incorporated into the LiNH2 lattice, which may affect the crystal morphology on the nano-scale.