Microstructured silicon (Si) materials have been fabricated by femtosecond (fs) laser ablation and have been hyperdoped with gold (Au) impurities. The ablated Si materials showed large and thermostable infrared absorption at 1.1–2.5 μm wavelengths, which was contributed by sub-band absorption and laser-induced defects absorption. The Au–Si alloy was formed after laser irradiation onto the Au-coated Si surface, which was determined by XRD characterization. Using N-type Si substrate, the fabricated Au-doped Si performed lower sheet carrier density due to the self-compensation effect between deep donor and acceptor energy lever of Au in bulk Si material. From Hall measurement, both the p- and n- types of Au-doped Si samples can be obtained by controlling the type of Si substrate.