An experimental investigation on synthesis of nanocrystalline nickels by pulsed current electrodeposition has been carried out in an additive-free Watts bath employing nickel-sulphate solution with similar nickel ion concentrations. Aluminum was used as a substrate. It demonstrated the advantage of easier removal process of electrodeposited nanocrystalline nickel from its substrate. Whereas the use of high-purity nickel anode was intended to replace nickel ions, which decreased during electrodeposition. Different peak current densities of 450, 750 and 1000 mA/cm2 were applied. A pulsed current was set at a similar pulse pattern of on-time and off-time of 1 ms and 9 ms respectively. The shorter on-time demonstrated the ability to limit ion deposition, which was related to the formation of finer grains. The off-time arrangement was targeted to ensure that the ion mobility had completely stopped. Higher current density demonstrated a dominant impact on deposits, generating a higher nucleation rate that is related to depositing nanocrystalline nickel. A peak current density of 1000 mA/cm2 produced grain sizes in the nanoscale regime. Without any additional additive, nanocrystalline nickel was successfully yielded. Investigation of grain size obtained from the 1000 mA/cm2 has been conducted by extracting full width at half maximum peak intensity (FWHM) revealed from X-ray diffraction (XRD) and Transmission Electron Microscopy (TEM) exhibited consistent results of 22 nm and 25.4±3.4 nm, respectively. It is also evidence of the significant role of pulsed current density. In inclusion, nanocrystalline nickel can be synthesized in an electrodeposition bath without any addition of additives