The influence of annealing time and annealing temperature under controlled partial pressure of selenium on the in-plane electrical transport properties of specimens of [(PbSe)0.99]1[WSe2]1 turbostratic nanolaminates was studied. The annealing treatments were found to be very effective in reducing carrier concentrations and improving carrier mobility in the annealed films, which is attributed to the reduction of compositional and structural defects. As a result, room temperature Hall mobilities greater than 60 cm2 V−1·s−1 are observed in spite of the small in-plane domain sizes (on the order of 10 nm) that are related to the turbostratic disorder. The technique appears promising for decreasing the concentration of kinetically trapped defects in these and related self-assembled nanostructures, a key challenge to evaluating the expected potential for controlling electrical and thermal transport properties via designed nanostructure in these and related materials.