Ni- and Co-based M–Cr–Al–Y (M = Ni and/or Co), dual phase β and γ/γ′, β—Ni–Al, γ—Ni(Co, Cr), and γ′—Ni3–Al superalloys exhibit several beneficial high-temperature (>1000 °C) (2012 °F) strength and corrosion resistance properties. Our study investigates the feasibility of fabricating a commercially available Ni–Co–Cr–AlY alloy (tradename “Amdry 386”) using laser directed energy deposition (laser-DED). A significant challenge for laser fabrication of bulk Amdry 386 (A386) structures stems from the presence of relatively higher amounts of the β phase than γ/γ′ phases. While prior studies report laser fabrication of these materials in coating and cladding configurations, bulk structures have not been realized. To investigate these challenges, this study was developed to systematically evaluate the effects of modifying the A386 alloy by adding 10, 20, and 30% by weight of a Ni–20%Cr (Ni–Cr) alloy (mainly γ/γ′). Laser-DED-fabricated A386 coupons exhibited a metastable, rapidly solidified β-rich microstructure typical to laser processes. The A386 + Ni–Cr mixtures were processed using laser-DED, and small coupons from each composition were evaluated using SEM, XRD, and microhardness to characterize the as-processed microstructure. Thermodynamic modeling was performed to determine the phase evolution as a function of the alloy composition. The dominating phase switches from β to γ/γ’ between the A386 and A386 + 10% Ni–Cr mixtures, but the increase in structural integrity is not observed until the Ni–Cr additions reach a minimum of 20%. Our results show that the alloy chemistry can be successfully modified to improve the structural integrity of laser-processed structures.