This study presents a comparative study on architecture‐dependent electrochemical properties of anodes made from aluminum particles and aluminum foil for lithium‐ion batteries (LIBs) application. The purity and other physicochemical features were analyzed by X‐ray diffraction (XRD), energy‐dispersive X‐ray spectroscopy (EDX), and scanning electron microscopy (SEM) methods. The electrochemical characteristics were determined by cycling voltammetry (CV) and galvanostatic charge/discharge (GCD) tests. The obtained results demonstrated that, due to the architecture nature of aluminum foil, the aluminum foil electrode had better conductivity and higher nucleation overpotential compared to the aluminum particles electrode, which involved other components such as PVDF as binder and carbon super P as conductive agent. Thus, the CV curves of the aluminum foil electrode showed sharper redox peaks with higher peak intensity. In addition, the aluminum foil electrode provided significantly higher initial capacity than that of the aluminum particles electrode. However, the architecture of the foil anode rendered it extremely prone to volume expansion during cycling, resulting in a fast and complete capacity fading just after 13 cycles. The anode made from aluminum particles, in contrast, witnessed slower capacity decay and ultimately stabilized at approximately 50 mAh g−1 for extending cycles.