Hybrid manufacturing, which, e.g., combines additive manufacturing with conventional machining processes, can be a way of overcoming limitations currently encountered in additive manufacturing. Cryogenic milling might be a viable option for hard-to-cut materials, as it leaves a contamination-free surface and can increase surface quality and tool life compared to conventional cooling concepts. In this study, the influence of cryogenic milling with carbon dioxide on titanium Ti-6Al-4V specimens manufactured with laser metal deposition (LMD) was investigated regarding tool wear and surface integrity in comparison to dry machining and machining with cooling lubricants. Moreover, additional layers of material were deposited on top of conventionally and cryogenically machined surfaces by means of LMD. The interface zone was then examined for defects. The milling process was closely monitored by means of thermal and high-speed imaging. Optical and tactile surface analysis provided evidence that lower roughness values and improved surface qualities could be obtained with cryogenic machining in comparison to dry machining. Moreover, significantly less tool wear was observed when a cryogenic cooling medium was applied. Although the utilization of conventional cooling lubricants resulted in satisfying surface qualities, substantial residual contamination on the milled surface was detected by means of fluorescence analysis. These contaminants are suspected to cause defects when the next layer of material is deposited. This is supported by the fact that pores were found in the weld bead applied on top of the milled specimens by means of LMD. Conversely, cryogenic machining resulted in very clean surfaces due to the residue-free evaporation of the coolant. Hence, a good metallurgical bonding between the weld bead and the milled substrate could be achieved. The results indicate the great potential of cryogenic milling in hybrid manufacturing, especially in terms of intermediate machining, as it provides residue-free surfaces for subsequent material deposition without an additional cleaning step and can significantly prolongate tool life.