With industrial developments of aerospace vehicles, marine devices, biomedical and bones, pure Ti and its alloys have gained a great deal of attraction due to their superior properties. Despite having promising properties, limitations of lower hardness, inferior weldability, and poor brittle fracture have restricted their applications. So the objective of this work was to make surface electrodeposition of nanocrystalline Ni coatings on the surface of TA2 substrate using pulsed electrodeposition. Scratch tests was used to compare how effects of two typical HF and DMF activating solutions on modifying interfacial adhesion between TA2 substrate and surface coatings. In order to disclose crystal growth of Ni coating without and with CeO₂ addition, a variety of characterizations such as FESEM, TEM and XRD were employed. A novel decussating-type microhardness with different loading forces attached with nanoindentation tests was conducted to make a comparative study of toughness and strengthening mechanisms between surface coatings and the un-coated TA2 substrate. Besides, wear behaviors of specimens was carried out using the ball-disc dry sliding tests. Results indicated that the addition of CeO₂ nanoparticles into electroplating solution has effectively modified textural growth of Ni grains. This result was attributed to the presence of nano-sized CeO₂ particles that adsorbed onto the preferred locations of crystal Ni growth, leading into an increasing catalytic site of nucleation to reduce Gibbs energy for grain refinement. According to observations of edges for hardness indentations, a smaller size with convergence feature for Ni-CeO₂ coatings was indicative of effects of CeO₂ nanoparticles or its precipiated Ce solute atoms on alloying-dispersion strengthening for completing defective grain boundaries. While for the case of a divergency state of indentations edges within obviously spalling cracks, it exhibited poor surface toughness for pure nickel. Furthermore, An analytic modeling validated here was based on the by-passing Orowan for dislocations pile-up mechanisms, in which this was contributed to the co-existence of Ce-rich worn products and NiO passive film to be expected as solid lubricants and make the self-lubricating effect, thereby improving wear resistance of Ti alloys where subjected to harsh conditions.