This study investigated the bath compositions and plating conditions and crystal structure used for achieving nickel-thallium-phosphorus deposits by means electroless plating. The electroless nickel-thallium-phosphorus deposits were achieved with a bath using sodium hypophosphite as the reducing agent and sodium citrate as the complexing agent. The depositing rate was 10.5mg.$cm^{2-1}$ .$hr^{-1 }$ from the optimistic bath composition, 0.1M nickel sulfate, 0.005M thallium sulfate, 0.2M sodium hypophosphite, and 0.05M sodium citrat and the recommended plating conditions, pH 5.5 and $90^{circ}C$. The composition of alloy deposits determined by X-ray analysis (EDS) that the Thallium was increased with major increasing concentration of complexing agent and thallium ion in bath solution, it decreased according to the increasing concentrations of reduction agent in the bath solution, Bit Phosphorus showed a contrary to the thallium. It was observed from X-ray diffraction analysis, Scanning Electron Microscopy and Transmission Electron Microscopy. The crystalline structure of deposits was amorphous at the first deposited state but it was changed $Ni-T1-Ni_{5}$ $P_2$ polycrystalline when subjected to 1 hour heat treatment of more than $350^{circ}C$. TEM observation demonstrated that the microstructure was identical to the result of the XRD at as deposited but it became $Ni-Tl-Ni_{5}$ $P_2$ polycrystalline when heated. And grain size was 10-50nm.