Laser metal deposition (LMD) has demonstrated its ability to produce complex parts and to adjust material composition within a single workpiece. It is also a suitable additive manufacturing (AM) technology for building up dissimilar metals directly. However, brittle intermetallic compounds (IMCs) are formed at the interface of the dissimilar metals fabricated by LMD. Such brittle phases often lead to material failure due to thermal expansion coefficient mismatch, thermal stress, etc. In this work, we studied a Fe-Ti system with two brittle phases, such as FeTi and Fe₂Ti, as a model system. Fe was grown on top of Ti at various process parameters. The morphologies and microstructures were characterized by optical microscopy (OM) and scanning electron microscopy (SEM). No cracks along the interface between pure Ti and bottom of the solidified melt pool were observed in the cross-sectional images. Chemical composition in the fabricated parts was measured by Energy-dispersive X-ray spectroscopy (EDS). Electron backscatter diffraction (EBSD) was performed in addition to EDS to identify the crystalline phases. The Vickers hardness test was conducted in areas with different phases. The chemical composition in the melt pool region was found to be a determining factor for the occurrence of major cracks.