Integrated Al/Ni electrodes of lithium-ion batteries (LIBs) with variant atomic ratios were successfully fabricated by a one-step laser-sintering process. The microstructure, phase composition, and pore structure were controlled by the raw material composition and laser parameters. The electrodes showed working merits without any conductive agent and binder, or even the collector used in a traditional battery. It was shown that the electrode consisted of multi-phases, i.e., Al, Al₃Ni₂, Al₃Ni, and Ni, when the Al/Ni atomic ratio was higher than 5 : 5. A lower Al/Ni atomic ratio less than 5 : 5 favored the formation of a dual-phase electrode consisting of Al₃Ni₂ and Ni. As the Al content increased, the specific surface area of the as-sintered electrodes increased in the initial stage and then decreased. The formation of pores was closely related to the content of the residual Al phase after the laser sintering. The residual Al phase filled the pores when the Al content was high, leading to a lower pore size. In contrast, the liquid Al phase completely reacted with the Ni component, leaving a large number of pores at its original sites. The linked pores can serve as transport channels for Li⁺ ions, provide mass sites for electrochemical reactions, and also buffer huge volume changes of the active material. Among the electrodes, the one with an Al/Ni ratio of 3 : 7 showed the best cycling/rate performance, i.e., a capacity of 522.8 mA h g⁻¹ by a current of 0.1 A g⁻¹ after 200 cycles, even holding to 338.4 mA h g⁻¹ by a big current impact at 2 A g⁻¹. It formed a metallurgical combination between the conductive network and the active material with multiple porous structures, which is helpful for the electrodes to provide high capacity and maintain structural stability during cycling. In addition, the average laser-sintering time of a single electrode was within 10 s, which is suitable for industrial mass production.