A wide variety of liquid and solid phase crystallized silicon films are investigated in order to determine the performance limiting defect types in crystalline silicon thin-film solar cells. Complementary characterization methods, such as electron spin resonance, photoluminescence, and electron microscopy, yield the densities of dangling bond defects and dislocations which are correlated with the electronic material quality in terms of solar cell open circuit voltage. The results indicate that the strongly differing performance of small-grained solid and large-grain liquid phase crystallized silicon can be explained by intra-grain defects like dislocations rather than grain boundary dangling bonds. A numerical model is developed containing both defect types, dislocations and dangling bonds, describing the experimental results. © 2014 AIP Publishing LLC.