Novel TiC-reinforced titanium matrix composites (TMCs) were in situ synthesized by laser powder bed fusion (LPBF) of unique carbon nanotube (CNT)-decorated Ti-6Al-4V powders. Acid-treated CNTs were coated on the surface of Ti-6Al-4V particles by electrostatic self-assembly without varying the powder sphericity, leading to improved printability, as proved by laser-absorption and single-track experiments. During L-PBF, the CNTs were completely transformed into monocrystalline TiC dispersed in the alpha'-Ti matrix via a dissolution/precipitation mechanism. As illustrated by high-resolution transmission electron microscopy, the in situ-synthesized TiC crystals were closely bonded to the matrix, exhibiting typical TiC [001]//Ti [00-1] and TiC (220)//Ti (-100) orientation relationships. Significantly, the morphology of TiC underwent an interesting evolution from nanorods to micro-spheres, and to dendrites with an increase in the CNT content, causing a gradual increase in hardness of TMCs. This study may provide insights into the design of high-performance TMCs with unique microstructures, excellent properties, and tailored architectures. (C) 2020 Elsevier B.V. All rights reserved.