Pulsed laser ablation (PLA) has several characteristics that are potentially attractive for the growth and doping of chemically complex compound semiconductors including (1) stoichiometric (congruent) transfer of composition from target to film, (2) the use of reactive gases to control film composition and/or doping via energetic-beam-induced reactions, and (3) low-temperature nonequilibrium phase formation in the laser-generated plasma “plume.” However, the electrical properties of compound semiconductors are far more sensitive to low concentrations of defects than are the oxide metals/ceramics for which PLA has been so successful. Only recently have doped epitaxial compound semiconductor films been grown by PLA. Fundamental studies are being carried out to relate film electrical and microstructural properties to the energy distribution of ablated species, to the temporal evolution of the ablation pulse in ambient gases, and to beam-assisted surface and/or gas-phase reactions. In this paper we describe results of ex situ Hall effect, high-resolution x-ray diffraction, transmission electron microscopy, and Rutherford backscattering measurements that are being used in combination with in situ RHEED and time-resolved ion probe measurements to evaluate PLA for growth of doped epitaxial compound semiconductor films and heterostructures. Examples are presented and results analyzed for doped II–VI, I–III–VI, and column-Ill nitride materials grown recently in this and other laboratories.