By using nc-Ni coatings as a model system, systematic experiments were designed to evaluate the interaction between the microstructural and mechanical properties tailored by electrodeposition conditions. A direct correlation between grain size and texture was established for the first time. The grain size of the (111) crystalline plane decreases with the texture coefficient (RTC) regardless of the process conditions, and that of the (220) plane has different trends. Then, a peculiar phenomenon is revealed that the dependence of hardness on grain size is accurately described by the Hall-Petch relationship when changing the temperature or pH, but with different slopes, while it deviates from such a relationship with changing current density, denoting more underlying mechanisms related to texture. Finally, a surprising degree of influence of texture on hardness and elastic modulus is also presented, with the overall trend of hardness increasing with texture; and when the RTC of (111) exceeds 40%, the elastic modulus increases with texture, implying a fundamental relationship between modulus and texture. Texture predominates over the other factors on the elastic modulus, revealing the importance of elastic anisotropy. Significantly, the present work suggests a useful tailoring routine to fabricate high quality nc-Ni coatings with the desired structure and mechanical properties.