Materials with high specific capacity, ultrahigh stability, and fast-charging capability are essential for the next-generation Li-ion batteries. To meet these demands, it is important to find alternative anode materials beyond graphite as it suffers from multiple challenges, such as low specific capacity, poor rate capability, and unstable behavior at high current densities. Nickel silicate hydroxides (NiSi) are a class of layered materials with high theoretical capacity, low cost, and high mechanical strength. However, they suffer from poor electronic conductivity, which hampers their cyclic stability at high current densities and limits their usage for fast-charging applications. Herein, NiSi grown over expanded graphite (EG) under in situ conditions (NiSi/EG composites) show superior electrochemical performance with ultrahigh stability of 3000 cycles at 1 A g