Amorphous thin films of AgInSe2 were grown by rf magnetron sputtering and then crystallized using two forms of optical annealing: laser annealing using a raster-scanned argon laser and heat-pulse annealing using a quartz–halogen heat-lamp system. It was determined that laser annealing of films on amorphous substrates resulted in fine-grained polycrystalline chalcopyrite AgInSe2 thin films with a preferred (112) orientation. The presence of weak X-ray diffraction peaks associated with nonchalcopyrite phases indicated that some segregation had occurred. Heat-pulse annealing of films on single-crystal substrates led to better results. The films were more highly oriented with no evidence of any segregation.