Heterostructured Cu2S-In2S3 nanocrystals with various shapes and compositions were synthesized by a high-temperature precursor-injection method using the semiconductor nanocrystal Cu1.94S as a catalyst. The intrinsic cationic deficiencies formed at high temperature by Cu ions made the Cu1.94S nanocrystal a good candidate for catalyzing the nucleation and subsequent growth of In2S3 nanocrystals, eventually leading to the formation of heterostructured Cu2S-In2S3 nanocrystals. Gelification of the reaction systems, which were composed of different types of nanocrystal precursors and solvent, was found to be a very effective measure for controlling the growth kinetics of the heterostructured particles. Consequently, matchsticklike Cu2S3-In2S3 heterostructured nanorods, teardroplike quasi-core/shell Cu2S@In2S3 nanocrystals, and pencil-like In2S3 nanorods were successfully obtained by manipulating the gelification of the reaction system; this formed a solid experimental basis for further discussion of the growth mechanisms for differently shaped and structured nanocrystals. By reaction with 1,10-phenanthroline, a reagent that strongly and selectively binds to Cu+, a compositional transformation from binary matchsticklike Cu2S-In2S3 nanorods to pure In2S3 nanorods was successfully achieved.