The Ni-based Hastelloy C-276 was repaired by in-air and underwater laser direct metal deposition (in-air DMD and UDMD) with four gradient cooling rates (in-air DMD, in-air DMD with interlayer cooling, UDMD and UDMD with each layer re-covered by water). The microstructure and mechanical properties of repaired samples were systematically characterized with respect to the cooling rates. All samples presented good metallurgical bonding and columnar dendrites with epitaxial growth. The underwater environment had a more pronounced acceleration effect on the cooling rate compared to interlayer cooling. The rapid cooling induced intense thermal cycling, resulting in increased dislocation density and grain refinement with primary dendrite arm spacing (PDAS) diminishing from 5.30 to 3.21 μm. Accelerated cooling rate contributed to precipitation of massive M6C carbides. Carbides coarsened (sizes from 257 to 354 nm) and exhibited a reduced content as cooling rate slowed down due to intrinsic heat treatment (IHT). The residual water film in UDMD repair promoted oxide formation. Samples with increased cooling rates exhibited superior mechanical performance. The improved microhardness, tensile and impact properties were primarily attributed to the enhanced fine grain strengthening and Orowan strengthening facilitated via reduced grain size, increased dislocation density and carbide content. Quantities of large-size carbides were detrimental to tensile and impact properties as displayed in the in-air DMD sample with interlayer cooling (carbide size of 341 μm). The study could serve as a reference for in-situ restoration in deep-water environments.