To assess the individual and synergistic effects of 2-butyne-1,4-diol (BD) and chloride ions on the microstructure and residual stress of electrodeposited nickel, various nickel layers were prepared from sulfamate baths comprising varying concentrations of BD and chloride ions by applying direct-current electrodeposition. And their surface morphologies, microstructure, and residual stress were tested using SEM, XRD, EBSD, TEM, and AFM. While the nickel layers composed of pyramid morphology were prepared from additive-free baths, the surface flattened gradually as the BD concentration of the baths was increased, and the acicular grains in the deposits were replaced with <100> oriented columnar grains or <111> oriented nanograins; additionally, the residual tensile stress of the deposits increased. The addition of chloride ions to the baths containing BD significantly increased the residual stress in the nickel layers, although it only slightly promoted surface flattening and columnar grain coarsening. The effects of BD and chloride ions on the growth mode and residual stress of nickel deposits were explained via analysis of surface morphologies and microstructure. And the results indicate that the reduction of chloride ion concentration is a feasible way to reduce the residual stress of the nickel deposits when BD is included in the baths.